The US actor, whose career stretched across 60-plus years, was described as the "quintessential chameleon" for the vast range of characters he has portrayed when he was given an honorary Oscar a little over three years ago.
New York-born Wallach notched up ten years as a stage actor, including Broadway success, before making his movie debut in 1956 in Baby Doll.
His film career also included appearances The Godfather: Part III, How The West Was Won and Mystic River. Wallach also had an extensive TV career and continued to draw acclaim for his stage work alongside his screen roles.
Despite his versatility, he acknowledged that he tended to be cast as a villain, saying in one interview: "As an actor I've played more bandits, thieves, warlords, molesters and mafioso than you could shake a stick at."
He continued to appear on screen into his 90s, including a role in the 2010 film The Ghost Writer which starred Ewan McGregor and Pierce Brosnan.
His daughter Katherine confirmed his death to the New York Times.