Other television work
After 77 Sunset Strip, Zimbalist appeared in other series, including CBS's short-lived The Reporter starring Harry Guardino as journalist Danny Taylor of the fictitious New York Globe. He also appeared in leading and supporting roles in several feature films, including Harlow, A Fever in the Blood (a film about a ruthless politician), Wait Until Dark and Airport 1975.
Zimbalist had a recurring role as Daniel Chalmers, a white-collar con man, on his daughter Stephanie Zimbalist's 1980s television detective series Remington Steele. He also recurred in the television dramatic series Hotel.
In 1990, Zimbalist portrayed the father of Zorro in the Christian Broadcasting Network's The New Zorro. Zimbalist relinquished the role after the program's first season because of the filming at studios outside Madrid, Spain, and the role subsequently went to Henry Darrow. He had a small recurring role in the 1990s hit science fiction television series Babylon 5 as William Edgars.
Also in the 1990s, Zimbalist voiced Alfred Pennyworth in Batman: The Animated Series. He reprised the role in subsequent media set in the DC Animated Universe, including Superman: The Animated Series, The New Batman Adventures, Justice League, and Static Shock. He said being Alfred had "made me an idol in my little grandchildren’s eyes.” Zimbalist also played villain Doctor Octopus in Spider-Man: The Animated Series. He appeared on the Trinity Broadcasting Network and as himself in the 1998 Smithsonian Institution production of Gemstones of America. He performed as the narrator in "Good Morning, America" by Elinor Remick Warren.
Zimbalist wrote an autobiography, My Dinner of Herbs, published by Limelight Editions, New York.
In 2008, Zimbalist appeared in the short film The Delivery, in which he played a professor who helps a young girl in her struggles for literacy. The film won first place in fantasy at the Dragon*Con Film Festival and was an official selection at the Los Angeles International Children's Festival and the Reel Women International Film Festival in 2009.
