The performer – real name Barry Elliott – starred alongside his younger brother Paul for more than 50 years.
The brothers were born in Rotherham, South Yorkshire, and first appeared on talent show Opportunity Knocks in 1967 before making their name with BBC show ChuckleVision in the 1980s and 1990s.
Paul, 70, said: "I've not just lost my brother, I've lost my theatrical partner of many, many years and my very best friend."
Manager Phil Dale added in a statement: "It is with great sadness that the family announce that Barry passed away peacefully at his home surrounded by his wife Ann and all his family.
"The family would like to express their thanks to the many people who have been fans of the Chuckle Brothers and they know that they will share in part the great, great loss they feel."
Barry had fallen ill while filming for a new Channel 5 show 'Chuckle Time' earlier this year and his condition deteriorated.
Their father James Elliott went by the stage name Gene Patton and worked the London club scene, even performing with an 18-year-old Peter Sellers in 1943.
Barry and Paul first broke onto the BBC in 1985 with the show Chuckle Hounds, which was aimed at pre-school children and saw the comedy duo dressed as dogs.
But they found fame with ChuckleVision, which became known for catchphrases such as 'To Me To You' and 'Oh dear, oh dear'.
The show claimed a Children's BAFTA among a host of awards and was one of the longest running children's programmes on the BBC, running from 1987 to 2009.
After it finished the pair made appearances in programmes such as The Weakest Link, Ant & Dec's Saturday Night Takeaway and Celebrity Coach Trip.
More recently they had been guests on Walliams and Friend and Blankety Blank in 2016 and The Nightly Show in 2017.
Their final TV appearances came in Chuckle Time, a clip show featuring the legendary pair, which saw filming stopped early due to Barry's ill health.
A host of stars joined fans in paying tribute to the star after the news broke this morning.
Take Me Out host Paddy McGuinness tweeted alongside a picture of Barry: "One of my favourites from childhood years, teenage years and as an adult! Gutted. Barry Chuckle RIP sir."
Actress Lisa Riley took to Instagram to write: "Dearest Barry, Rest in Peace, do what you do so well, make all the angels you now join happy and make them always laugh.
"You know how much I adore you and ALL your family. @PaulChuckle2 stay strong, with your memories of LAUGHTER through this tough time #tometoyou."
Fellow boxing legend Frank Bruno tweeted: "Very sad news this morning. A very funny man, you've left happy memories for so many people 'to me to you' RIP #barrychuckle."
Meanwhile many celebrities revealed their love for Chucklevision when they were growing up.
Blue's Antony Costa tweeted: "#BarryChuckle R.I.P loved watching him and @PaulChuckle2 when I was younger on chucklevision…and had the please of working with him on celeb juice…such a lovely bloke."
The BBC's Dan Walker added: "How very sad. Huge part of so many childhoods. Friendly, daft and they genuinely used to make me laugh. To you, Barry."
EastEnders actress Bonnie Langford wrote: "This is so sad to hear. Such a lovely man. Love and hugs to Paul and the family xx."
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