| Brian T. Delaney | .. | Player Male (voice) |
| Courtenay Taylor | .. | Player Female (voice) |
| Stephen Russell | .. | Nick Valentine / Mr. Handy / Codsworth / Atomic Dreamz / Bean / Bob's Your Uncle / Bosun / Cook Handy / Crisp / Danny / Deezer / Fusion's Folly / Goodfeels / Kingpin / Lookout / Mack / Maxwell / Mr. Navigator / Old Rusty / Percy / Piece O'Junk / Reg / Split / Sprocket / Strike / Supervisor Brown / Supervisor Greene / Supervisor White / The Champ / Tenpin / Torte / Waitron / Wellingham / Whitechapel Charlie / DiMA - Far Harbor DLC (voice) |
| Courtney Ford | .. | Piper Wright (voice) |
| Peter Jessop | .. | Paladin Danse (voice) |
| Jon Gentry | .. | Preston Garvey (voice) |
| Claudia Christian | .. | Desdemona / Mrs. Whitfield / Mistress Mysterious (voice) |
| Ryan Alosio | .. | Deacon / H2-22 (voice) |
| Danny Shorago | .. | Hancock (voice) |
| Katy Townsend | .. | Cait (voice) |
| Matthew Mercer | .. | MacCready / Z1-14 (voice) |
| Sophie Cortina | .. | Curie / Miss Edna (voice) |
| David Paluck | .. | X6-88 (voice) |
| Sean Schemmel | .. | Strong / Male Ghoul (voice) |
| Brendan Hunt | .. | Travis Miles / Perry (voice) |
| Tony Amendola | .. | Father / Colonel Smith / Josh (voice) |
| Derek Phillips | .. | Elder Maxson / Z2-47 (voice) |
| Ron Perlman | .. | Anchorman (voice) |
| Lynda Carter | .. | Magnolia (voice) |
| Kari Wahlgren | .. | Proctor Ingram (voice) |
| Tim Russ | .. | Lancer Captain Kells (voice) |
| Jonathan Roumie | .. | Jack Cabot / Doc Weathers / Honest Dan (voice) (as Johnathan Roumie) |
| Jan Johns | .. | Scribe Haylen / Ellie Perkins / Colette / Sierra Petrovita (voice) |
| Jennifer Massey | .. | Madison Li (voice) |
| Matthew Waterson | .. | Virgil (voice) |
| Byron Marc Newsome | .. | Tinker Tom (voice) |
| Nicholas Guy Smith | .. | Proctor Quinlan / Supervisor Brown (voice) |
| Philip Anthony-Rodriguez | .. | Sturges / Scott Edwards (voice) |
| Jerry Whiddon | .. | Henry Cooke / Bert Strickland (voice) |
| Noshir Dalal | .. | Knight Rhys (voice) |
| Elisabeth Noone | .. | Ronnie Shaw / Irma (voice) |
| T.W. Leshner | .. | Paul Pembroke / Neil Freund (voice) |
| Roberta Farkas | .. | Bobbi No-Nose / Maria Summerset (voice) |
| Meher Tatna | .. | Doctor Amari (voice) |
| Clarke Kohler | .. | Tommy Lonegan (voice) |
| Sean T. Krishnan | .. | Doctor Carrington (voice) |
| William Holmes | .. | Edward Deegan / AJ (voice) (as Bill Holmes) |
| Colleen Delany | .. | P.A.M. / Assaultron (voice) |
| Chelsea Tavares | .. | Glory (voice) |
| Greg Baldwin | .. | Proctor Teagan (voice) |
| Matthew Yang King | .. | Justin Ayo / Male Raiders (voice) |
| Dwight Schultz | .. | Knight Captain Cade (voice) |
| Maya Massar | .. | Mama Murphy (voice) |
| Ellen Dubin | .. | Alana Secord / Allie Filmore (voice) |
| Christopher Crutchfield Walker | .. | Initiate Clarke (voice) (as Christopher Walker) |
| Keythe Farley | .. | Kellogg / Y9-15 / X9-27 (voice) |
| Mike Rosson | .. | Minutemen Radio Voice / Vault-Tec Scientist (voice) |
| Finneas O'Connell | .. | Liam Binet (voice) |
| Dave Carter | .. | Mel / Super Mutants (voice) |
| Jay Giannone | .. | Kent Connolly / Eddie Winter (voice) |
| Dimitri Diatchenko | .. | Vadim Bobrov (voice) |
| Emmanuel Todorov | .. | Yefim Bobrov (voice) |
| Cindy Robinson | .. | Gwen McNamara / Becky Fallon (voice) |
| James Sie | .. | Jun Long / Doctor Sun (voice) |
| Jack Riedy | .. | Austin Engill / Chris Rosa / Pete Pembroke (voice) |
| Brandon Bales | .. | Bobby De Luca / Lucas Miller (voice) |
| Robert Picardo | .. | Alan Binet / Vault-Tec Scientist (voice) |
| Kat Cressida | .. | Scribe Neriah / Geneva (voice) |
| Elmarie Wendel | .. | Mandy Stiles / Cathy / Pulowski Voice (voice) |
| Audrey Wasilewski | .. | Alexis Combes / Darcy Pembroke / Female Child of Atom (voice) |
| Melendy Britt | .. | Ann Codman / Priscilla Penske / Wilhelmina Cabot (voice) |
| Dave Fennoy | .. | Max Loken / Malcolm Latimer (voice) |
| Alan Oppenheimer | .. | Paladin Brandis (voice) |
| Paul Eiding | .. | Vault-Tec Rep / Arlen Glass (voice) |
| Charlie Warren | .. | Mayor McDonough (voice) |
| Wes Johnson | .. | Moe Cronin / Protectron / The Silver Shroud / Takahashi / Buddy / FirstMate / Boson / Tin Man / Ironsides / Gus / Sarge / Sentry Bots / Super Mutant / Ahab - Automatron DLC (voice) |
| Caleb Moody | .. | Scribe Faris / Clayton Holdren (voice) |
| Ping Wu | .. | Captain Zao / Ted Huntley / Stan Slavin (voice) |
| Misty Lee | .. | Talia McGovern / Molly / Settler (voice) |
| Ashly Burch | .. | Tina De Luca / Rowdy / Cricket (voice) |
| Richard Cansino | .. | Ricky Dalton / Solomon / Lorenzo Cabot (voice) |
| Iona Morris | .. | Daisy / Cheryl Glass / Clair Hutchins / Gibson (voice) |
| Eric Morgan Stuart | .. | Jacob Forsythe / Newton Oberly (voice) |
| Dani Knights | .. | Emogene Cabot / Pvt Hart / Amelia Stockton (voice) |
| Sumalee Montano | .. | Rachel / Female Gunners / Institute Scientist (voice) |
| Kyle Hester | .. | Pickman / Brother Andrew / Brother Thomas / Mayor Murphy (voice) |
| James Konicek | .. | Institute Courser / Doc Crocker / The Fens Phantom (voice) |
| Richard Tatum | .. | Rex Goodman / Vault-Tec Scientist / Isaac Karlin (voice) |
| Carla Tassara | .. | Knight Lucia / Katherine Pinn (voice) |
| Charles Halford | .. | Knight Gavil / Winlock (voice) |
| Time Winters | .. | Mister Zwicky / Old Man Stockton / Barney Rook (voice) |
| Salli Saffioti | .. | Female Raiders / Alyssa Park / Female Synths (voice) |
| Amanda Philipson | .. | Professor Scara / Smiling Kate / Trader Rylee (voice) |
| Greg Chun | .. | Marowski / Vault-Tec Scientist (voice) |
| Alan Blumenfeld | .. | Skinny Malone / Evan Watson / Clarence Codman (voice) |
| Roger Jackson | .. | Lawrence Higgs / Institute Scientist (voice) (as Roger L. Jackson) |
| Joan Van Ark | .. | Bonnie Tournquist / Phyllis Daily / Roslyn Chambers (voice) |
| Gustavo Rex | .. | Arturo / Enrico Thompson (voice) |
| Jacqueline Grace Lopez | .. | Ness / Rosalind Orman (voice) |
| Rachel Pace | .. | Erin Combes / Female Brotherhood of Steel Squire (voice) |
| Aidan Sussman | .. | Synth Child (voice) |
| Jessica Straus | .. | Supervisor White / Polly (voice) |
| Cissy Jones | .. | Doctor Duff / Doctor Patricia (voice) |
| Don McManus | .. | Wallace / John (voice) |
| Llou Johnson | .. | Pastor Clements (voice) (as Big Llou Johnson) |
| Max Mittelman | .. | Zeke / Brendan Volkert / Northy (voice) |
| Dan Navarro | .. | Jacob Orden / Dean Volkert (voice) |
| Avery Kidd Waddell | .. | Hawthorne / Low Road Franklin / Horatio (voice) |
| Christopher Salazar | .. | Sergeant Lee / Caretaker / Swanson (voice) (as Chris Salazar) |
| Yuri Lowenthal | .. | Danny Sullivan / Vault-Tec Scientist (voice) |
| Rafael Goldstein | .. | Henri / Fred Allen / Fat Fahey (voice) |
| Alejandra Gollas | .. | Marcy Long / Myrna (voice) |
| Ogie Banks | .. | Holt Combes / Nelson Latimer / Preston Garvey Impersonator (voice) |
| Brenda Marie Phillips | .. | Scarlett / Anne Hargraves / Knight Astlin (voice) (as Brenda Phillips) |
| Julie Nathanson | .. | Maria / Penny Fitzgerald (voice) |
| John Mariano | .. | Abbot / Mark Summerset (voice) |
| J.P. Giuliotti | .. | Manny / Diamond City Guard (voice) |
| Brian Frates | .. | Supervisor Greene / Blake Abernathy / Joe Savoldi / Male Bostonian (voice) |
| William Salyers | .. | Bullet / Calvin Whitaker / Sheffield (voice) |
| Ike Amadi | .. | Davies / Diamond City Guard (voice) |
| Nick Bennett | .. | Theodore Collins / Blythe / Knight Varham (voice) |
| Erica Luttrell | .. | Darla / Fahrenheit / Kendra (voice) |
| Bruce Nozick | .. | Pete Owens / Male Gunners / Eye Bot (voice) |
| Damian Cecere | .. | F6-33 / X4-18 / Z3-22 (voice) |
| Stephanie Komure | .. | Miranda Song / K1-98 / Runaway Girl (voice) |
| Leo Marks | .. | Male Brotherhood of Steel / Triggerman (voice) |
| Joey Honsa | .. | Angie / Eleanor / Kessler (voice) |
| Bruce Thomas | .. | Daniel Finch / Nathan Filmore / Drifter (voice) |
| Mandy Kaplan | .. | Connie Abernathy / June Warwick / Settler (voice) |
| Veronica Cartwright | .. | Trashcan Carla / Doc Anderson / Principal Hudson (voice) |
| Jim Cummings | .. | The Scribe / Institute Scientist (voice) |
| Miya Horcher | .. | Marlene Glass / Alice Thompson / Child (voice) |
| Griffin Cleveland | .. | Wally Warwick / Gavin Everitts / Child (voice) |
| Kimberly Brooks | .. | Female Brotherhood of Steel (voice) |
| Dorothy Elias-Fahn | .. | Female Brotherhood of Steel / Vault-Tec Scientist (voice) |
| Mark Engelhardt | .. | Male Brotherhood of Steel (voice) |
| Popeye Vogelsang | .. | Super Mutant / Officer (voice) (as Popeye V) |
| Steve Wilcox | .. | Male Raider (voice) |
| Gabrielle Sanalitro | .. | Female Ghouls (voice) |
| Keith Szarabajka | .. | Male Ghouls / Vault-Tec Scientist / John-Caleb Bradberton - Nuka-World DLC (voice) |
| Dave B. Mitchell | .. | Male Gunners / Mr. Gutsy (voice) (as David B. Mitchell) |
| Paul Ganus | .. | Male Children of the Atom (voice) |
| Joe Ochman | .. | Male Child of Atom / Vault Security (voice) |
| Brandon Keener | .. | Sully Mathis / Drummer Boy / Rufus Rubins / Settler / Railroad Agent / Initiate / Phil Roller - Nuka-World DLC (voice) |
| Fryda Wolff | .. | Vault Security (voice) |
| Raymond Ochoa | .. | Male Brotherhood of Steel Squire (voice) |
| Kevin Dorman | .. | Air Traffic Control Voice (voice) |
| Lyne Odums | .. | Eustace (voice) (as Baadja-Lyne Odums) |
| Eric Lopez | .. | Mr. Washington (voice) |
| Colleen O'Shaughnessey | .. | Sylvia Cooper (voice) |
| David Shaughnessy | .. | General Gage / Mayor (voice) |
| Wayne Frazier | .. | Gerald / Wicked Tim (voice) |
| River | .. | Dogmeat (voice) |
| Cindy Richardson-Walker | .. | Singer (voice) |
| Tanya Hancheroff | .. | Singer (voice) (as Tania Hancheroff) |
| Lisa Silver | .. | Singer (voice) |
| Bumper Robinson | .. | Additional Voices (voice) |
| Billy Ray Gallion | .. | Additional Voices (voice) |
| Caroline Aaron | .. | Additional Voices (voice) |
| James McDonnell | .. | Additional Voices (voice) |
| Patrick FitzSymons | .. | Additional Voices (voice) |
| Ray Chase | .. | Additional Voices (voice) |
| Taliesin Jaffe | .. | Automatron - Automatron DLC (voice) |
| Stephanie Lemelin | .. | The Mechanist - Automatron DLC (voice) |
| Rachel Robinson | .. | Ada - Automatron DLC (voice) |
| Dan Donohue | .. | High Confessor Tektus - Far Harbor DLC (voice) |
| Crispin Freeman | .. | Brooks - Far Harbor DLC / William Moseley - Far Harbor DLC / Andre Michaud - Far Harbor DLC (voice) |
| Mimi Torres | .. | Kasumi Nakano - Far Harbor DLC (voice) (as Megan Goldsmith) |
| Haviland Stillwell | .. | The Mariner - Far Harbor DLC (voice) |
| Michelle Wong | .. | Sister Mai - Far Harbor DLC / Rei Nakano - Far Harbor DLC (voice) |
| Sam Riegel | .. | Brother Devin - Far Harbor DLC / Cole - Far Harbor DLC / Faraday - Far Harbor DLC (voice) |
| Liam O'Brien | .. | Allen Lee - Far Harbor DLC / Keith McKinney - Far Harbor DLC (voice) |
| Chris Andrew Ciulla | .. | Machete Mike - Far Harbor DLC / Malcolm - Far Harbor DLC (voice) |
| Erika Harlacher | .. | Sister Gwyneth - Far Harbor DLC (voice) |
| Karen Strassman | .. | Overseer Barstow - Vault-Tec Workshop DLC (voice) |
| Anjali Bhimani | .. | Nisha - Nuka-World DLC (voice) |
| Ivan Dixon | .. | Bottle - Nuka-World DLC / Cappy - Nuka-World DLC (voice) |
| Laura Post | .. | Mags Black - Nuka-World DLC (voice) |
| Mark Rolston | .. | Porter Gage - Nuka-World DLC (voice) |
| Rest of cast listed alphabetically: |
| Orion Acaba | .. | Operators / Additional Voices |
| Krizia Bajos | .. | Additional Voices (voice) |
| Stephen Ellis | .. | Scientist (voice) |
| Corri English | .. | Shelbie Chase (voice) |
| Pat Fitz | .. | Multiple Voices (voice) |
| Daniel Giordano | .. | Male Brotherhood of Steel (voice) |
| Shinji Mikami | .. | Takahashi (voice) |
| Jean Louise O'Sullivan | .. | Victory Girl (voice) |
| Scott von Berg | .. | Super Mutant / Diamond City Guard (voice) |
| Robin Atkin Downes | .. | Finn / Sinjin (voice) (uncredited) |
| Franciska Friede | .. | 'Katy' Katherine Pinn (German voice) (voice) (uncredited) |
| Paul Skinner | .. | Wilson / Additional Voices (voice) (uncredited) |
| Lars Slind | .. | Brotherhood of Steel Paladin (voice) (uncredited) |
| Andrew W.K. | .. | RedEye - Nuka World DLC (voice) (uncredited) |
