He earned his first Oscar nomination for Judah Rosenthal in Crimes & Misdemeanors with a Best Supporting Actor nod, an award he won in 1994 for Ed Wood.
But during career doldrums, the New York-born Landau languished in third-rate projects such as the laughable 1981 TV movie The Harlem Globetrotters on Gilligan's Island and the dispensable 1983 mutant monster movie The Being.
Following his Oscar win, Landau remained prolific, with roles in the likes of City Hall, The X-Files, Rounders, The Majestic, Hollywood Homicide and Frankenweenie.
Normality for Landau meant he never became a Hollywood A-lister, but he saw a benefit in not being a highly sought-after actor.
He was Star Trek creator Gene Roddenberry's first pick to portray pointy-eared Mr Spock.
After a brief but impressive Broadway career, Landau had made an auspicious film debut in the late 1950s, playing a soldier in "Pork Chop Hill" and a villain in the Alfred Hitchcock classic "North By Northwest". Landau would finally strike Oscar gold (as well as his third Golden Globe, a BAFTA nomination, and a Saturn Award), winning acclaim for his portrayal of Bela Lugosi in Tim Burton's biopic Ed Wood (1994).
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Landau - who was hired at age 17 as a cartoonist at the New York Daily News, a resume tidbit that never ceases to delight me - had an acting career that stretched over six decades, moving back and forth between film and television as the opportunities allowed.
Since then, Landau had worked steadily in film, including starring opposite Paul Sorvino in "The Last Poker Game", which premiered at the 2017 Tribeca Film Festival in NY. The actor also starred in the television show "Mission Impossible".
It was in this drama that he was discovered by Hitchcock, who cast him as a killer, who falls to his death off Mount Rushmore, in North by Northwest.
Landau and Bain left the show in 1969, working together again in the cult English sci-fi series Space: 1999 in the mid-70s.
In a 2011 TV interview, he said, "I turned down Star Trek".
He is survived by his two daughters, a granddaughter and one sister. Or I was getting up to bat and no one was pitching to me.