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Several famous actors of film and video games lent their voices to Fallout 3, including Liam Neeson as James, Ron Perlman as the game's narrator, Malcolm McDowell as President John Henry Eden, and Odette Yustman as Amata Almodovar. Veteran voice actors Dee Bradley Baker, Wes Johnson and Stephen Russell also provided voice overs for the game.

The Fallout 3 soundtrack continued the series' convention of featuring sentimental 1940s big band American popular music, the main theme, and few other side songs recorded by The Ink Spots and the Andrews Sisters; in addition to a score written by composer Inon Zur. In a review of the game for Kotaku, Mike Fahey commented that "While Inon Zur's score is filled with epic goodness, the real stars of Fallout 3's music are the vintage songs from the 1940s."

The following is a list of the 20 licensed songs that appear in Fallout 3.

1. "I Don't Want To Set The World On Fire" The Ink Spots 3:07
2. "Anything Goes" Cole Porter 3:04
3. "A Wonderful Guy" Tex Beneke 2:48
4. "Boogie Man" Sid Phillips 2:23
5. "Butcher Pete (Part 1)" Roy Brown 2:28
6. "Crazy He Calls Me" Billie Holiday 3:05
7. "Civilization" Danny Kaye with The Andrews Sisters 3:07
8. "Easy Living" Billie Holiday 3:06
9. "Fox Boogie" Gerhard Trede 3:16
10. "Happy Times" (From the Danny Kaye film The Inspector General) Bob Crosby & the Bobcats 2:45
11. "I'm Tickled Pink" Jack Shaindlin 1:52
12. "Into Each Life Some Rain Must Fall" Ella Fitzgerald with The Ink Spots 3:06
13. "Jazzy Interlude" Billy Munn 2:52
14. "Jolly Days" Gerhard Trede 1:40
15. "Let's Go Sunning" Jack Shaindlin 1:41
16. "Maybe" (Intro song from the original Fallout) The Ink Spots 3:06
17. "Mighty Mighty Man" Roy Brown 2:36
18. "Rhythm for You" Eddy Christiani & Frans Poptie 2:59
19. "Swing Doors" Allan Gray 2:59
20. "Way Back Home" Bob Crosby & the Bobcats 2:54