The actor played Inspector Lewis Erskine in the show, which ran from 1965 until 1974.
Before that Efrem Zimbalist Jr. became a household name in the US playing private investigator Stu Bailey in 77 Sunset Strip, which ran from 1958 to 1964.
In later life he retired to his ranch in Solvang, California, where he died on Friday.
Efrem Zimbalist’s daughter Stephanie Zimbalist and son Efrem Zimbalist III said in a statement: “We are heartbroken to announce the passing into peace of our beloved father, Efrem Zimbalist Jr., at his Solvang ranch.
“He actively enjoyed his life to the last day, showering love on his extended family, playing golf and visiting with close friends.”
In addition to his leading TV roles, Efrem Zimbalist Jr. made numerous stage and film appearances. His stage debut was opposite Spencer Tracy in The Rugged Path.
His show The FBI was famous for posting real photos from the federal crime investigation agency’s most-wanted list at the end of each program.
The FBI honored Efrem Zimbalist Jr. by making him an honorary “G-man” in 2009.
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