Lloyd came to public attention in Northeastern theater productions during the 1960s and early 1970s, earning Drama Desk and Obie awards for his work. He made his cinematic debut in One Flew Over the Cuckoo's Nest (1975) and went on to star as Commander Kruge in Star Trek III: The Search for Spock (1984), Professor Plum in Clue (1985), Judge Doom in Who Framed Roger Rabbit (1988), Uncle Fester in The Addams Family (1991) and its sequel Addams Family Values (1993), Switchblade Sam in Dennis the Menace (1993), Mr. Goodman in Piranha 3D (2010), Bill Crowley in I Am Not a Serial Killer (2016) and David Mansell in Nobody (2021).

He earned a third Emmy for his 1992 guest appearance as Alistair Dimple in Road to Avonlea (1992), and won an Independent Spirit Award for his performance in Twenty Bucks (1993). He has done extensive voice work, including Merlock in DuckTales the Movie: Treasure of the Lost Lamp (1990), Grigori Rasputin in Anastasia (1997), the Hacker in the PBS Kids series Cyberchase (2002–present), which earned him Daytime Emmy nominations, and the Woodsman in the Cartoon Network miniseries Over the Garden Wall (2014).

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