- Sarita Choudhury - Lee Moldaver
- Leslie Uggams - Betty Pearson
- Michael Cristofer - Elder Cleric Quintus
- Johnny Pemberton - Thaddeus
- Mykelti Williamson - Honcho
- Zach Cherry - Woody Thomas
- Annabel O'Hagan - Stephanie Harper
- Dave Register - Chet
- Rodrigo Luzzi - Reg McPhee
- Cameron Cowperthwaite - Monty
- Jacinto Taras Riddick - Cleric Felix
- Joel Marsh Garland - Biggie
- Mike Doyle - Bob Spencer
- Janie Brookshire - Mrs. Spencer
- Leer Leary - Davey
- Jacob A. Ware - Slim
- Brendan Burke - Officer Shortsight
- Jamal Thomas - Frank
- Logan Crawford - News Anchor
- Cedric Cannon - Elderly Speaker
- Tom DiNardo - Vault 32 Raider
- Luciana VanDette - Young Lucy MacLean
- Mason Cufari - Roy Spencer
- Michael Emerson - Wilzig
- Dale Dickey - Ma June
- Jon Daly - Snake Oil Salesman
- Michael Abbott Jr. - Farmer
- Edythe Jason - Barv
- Jake Garber - Chicken Collector
- Martin Pfefferkorn - Filly Vendor #1
- David Bluvband - Filly Vendor #2
- Julian Rozzell Jr. - Filly Vendor #3
- Bari Hyman - Filly Vendor #4
- Frances Turner - Barb Howard
- Ash McNair - Emil Dale
- Nina Kassa - Sarah Clements
- Joe Castle Baker - George Yaffe
- Roberto De Felice - Jorge the Villain
- Matt Berry - Sebastian Leslie
- Matt Berry - Snip Snip (voice)
- Matt Berry - Mr. Handy (voice)
- Daniel Danielson - Vault 33 Engineer
- Michael Rapaport - Knight Titus
- Kyle MacLachlan - Overseer Hank MacLean
- Neal Huff - Roger
- Matthew Cardarople - Huey
- Danielle Alonzo - Veronica
- Peter Brensinger - Freed Ghoul
- Alexa Marcigliano - Martha
- Scott Hoffman - Feral Ghoul
- A.J. Paratore - Vault 33 Dweller
- Mitzi Akaha - Rink
- Nicholas Michael McGovern - Javin
- Evan Dane Taylor - Scavenger
- Chris Parnell - Overseer Benjamin
- Michael Esper - Bud Askins
- Michael Esper - Bud Askins / Brain-on-a-Roomba
- Cherien Dabis - Birdie
- Glenn Fleshler - Sorrel Booker
- Dallas Goldtooth - Charles Whiteknife
- Eric Berryman - Lloyd Hawthorne
- Angel Desai - Cassandra Hawthorne
- Harry Sutton Jr. - Dr. 'Nose' Edmundson
- Chip Carriere - Nurse Powell
- Vick Krishna - Friendly Vault 4 Dweller #1
- Zeby Khan - Party Guest #1
- David Denowitz - Party Guest #2
- Morgen McKynzie - Female Server
- Michael C. Brennan - Administrator
- Michael C. Brennan - Hank MacLean Stunt Double
- Mohammed J. Ali - Vault 4 Dweller
- Neimah Djourabchi - Vault 4 Dweller
- Fred Armisen - DJ Carl
- Erik Estrada - Adam
- Charlie Besso - Tommy
- Paul Mauriello - Angry Vault 4 Dweller
- Michael Mulheren - Frederick Sinclair (Big MT)
- Anthony Misiano - Robert House (RobCo)
- James Yaegashi - Leon Von Felden (West-Tek)
- Rebecca Watson - Julia Masters (REPCONN)
- Collin Ware - Chanting Cleric
- Justice Hedenberg - The Ghoul Stunt Double
- Hannah Scott - Lucy MacLean Stunt Double
- Danny Schoch - Biggie Stunt Double
- Samantha MacIvor - Ma June Stunt Double
- Brandon McClary - Dr. 'Nose' Edmundson Stunt Double
- Brandon McClary - Honcho Stunt Double
- Akos Schenek - Slim Stunt Double
- Akos Schenek - Javin Stunt Double
- Noreen O'Toole
- Jonathan Nolan
- John Papsidera
- Kim A. Winther
- Athena Wickham
- Halle Phillips
- Ramin Djawadi
- Trygge Toven
Mykelti Williamson interpreta a Honcho en la serie.
Michael Rapaport interpreta a Knight Titus en la serie.
Michael Emerson hace el papel de Wilzig.
Ella Purnell hace el papel de Lucy MacLean.
Aaron Moten interpreta a Maximus en la serie.
Moisés Arias interpreta a Norman 'Norm' MacLean en la serie.
Walton Goggins hace el papel de The Ghoul / Cooper Howard.
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