The retired teacher and his wife June were one of the first couples to join the show's cast when it launched in 2013.
In a statement on behalf of Bernicoff's family, Channel 4 and production company Studio Lambert said: "It is with a heavy heart that we announce the sad news that after a short illness Gogglebox's Leon Bernicoff passed away in hospital earlier today.
"Leon and his wife June were the first members of the public to be cast for Gogglebox back in early 2013, and they soon grew to become much-loved voices during the course of the show's 10 series to date.
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"Leon's unique personality and sharp wit endeared him to fans of the show, as he contributed fully to Gogglebox's reputation as a programme full of warm humour and unvarnished opinion.
"To those of us that knew him personally, Leon was a man of unwavering principles who exerted a distinct paternal presence both on and off screen. He will be dearly missed by the entire Gogglebox family; cast and crew.
"Our thoughts are with June, his two daughters, sons-in-law and beloved grandchildren – all of whom have asked for their privacy to be respected at this incredibly sad time."
“He will be dearly missed by the entire Gogglebox family, cast and crew.”
Studio Lambert spokesperson
Leon captured the nation's heart with his outspoken commentaries on the fly-on-the-wall show.
The Liverpool-based duo enjoyed over 60 years of marriage, with a 20-year-old Leon meeting June when she was just 18.
They first locked eyes at a teacher training college dance, admitting it was love at first sight.
TWITTER @LEONANDJUNE
However, apparently Leon's Jewish family had strong opinions about June's Catholic upbringing.
"My parents in particular resented it," he told The Daily Record.
"It was heartbreaking. We ended up having a very unromantic proposal. June was screaming at me saying, 'Are you going to marry me or not?' It was awful."
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June explained: "I knew our parents would accept us more if we were serious, and I wanted to make us official.
"So that was that. We had a small wedding that wasn’t fancy, it didn’t need to be.
"It was just about us. Even my dress was very ordinary."
TWITTER @LEONANDJUNE
Speaking about the secret to a happy marriage, Leon told The Mirror: "I just love her. I don’t know, that’s all I can say.
"When I come home and she smiles at me at the front door, well, it melts me. It’s lovely.
"I don’t want anybody else, only June."
Everton supporter Leon made headlines for his no-nonsense political commentary, famously branding Nigel Farage a "d***head" during a Brexit debate.