David McCallum, widely recognized for his decades-long career in live-action television and film, also built a substantial body of work as a voice actor in animated series and movies, particularly within the DC Universe animated franchise. His voice acting career, which he developed alongside his on-screen performances, included roles in major animated projects during the 2000s and 2010s.

McCallum is most notably remembered in animation for voicing Alfred Pennyworth, the trusted butler of Bruce Wayne. He first took on this role in the 2008 anime-influenced direct-to-video film Batman: Gotham Knight, an anthology piece set between the live-action films Batman Begins and The Dark Knight. He reprised the character of Alfred in two subsequent DC Universe Animated Original Movies, Son of Batman in 2014 and Batman vs. Robin in 2015.

Beyond the character of Alfred, McCallum voiced other significant figures in DC animated productions. In 2008, he appeared in the Batman: The Brave and the Bold television series, providing the voice for the legendary wizard Merlin in the episode Day of the Dark Knight. The following year, in 2009, he lent his voice to the king of the gods, Zeus, in the animated film Wonder Woman.

Outside of the DC Comics universe, McCallum's voice acting included a recurring role in the Ben 10 franchise. He voiced the character Professor Paradox, a time-displaced scientist, appearing in the Ben 10: Alien Force series and its related video game, Cartoon Network Universe: FusionFall. He also provided the voice for C.A.R.T.E.R., the sentient family car, in the Disney animated series The Replacements. His work in video games extended to the fantasy role-playing genre, where he voiced characters in Diablo III: Reaper of Souls.