Zorich was born in Chicago, Illinois, the son of Yugoslavian immigrants Anna (née Gledi) and Christ Zorich. He attended Earle Elementary School before going on to attend Roosevelt College and Goodman Theater School of Drama in his hometown of Chicago. Zorich has been married to Academy Award winning actress Olympia Dukakis since 1962. They have three children together.
In 1965, Zorich recorded and released an album on Folkways Records, entitled Moby Dick: Selections Read by Louis Zorich. One of Zorich's first major film roles was the Russian Constable in the 1971 film Fiddler on the Roof. He was featured in Popi and For Pete's Sake and played the role of Pete in the 1984 film The Muppets Take Manhattan. In 1986 he played a Swiss businessman in Club Paradise with Robin Williams, and in 1988 appeared as Nikos, the Greek millionaire, part of a group arriving in a yacht party, in Dirty Rotten Scoundrels (film) with Steve Martin and Michael Caine.