The 48-year-old comedian, who has hosted the popular Channel 4 show alongside Noel Fielding for three series, explained he was leaving as he could no longer commit to the programme's schedule alongside his other projects, including his new hosting role on the revived comedy show Fantasy Football League.
In an Instagram post on Tuesday, he wrote: "Farewell Bake Off! It's been a delicious experience and I can't imagine a more fun way of spending my summers.
"But it's become clear to me that I can't present both Fantasy Football League and Bake Off alongside all my other projects.
"So, after three series and 51 episodes, I am cheerfully passing the baguette on to someone else.
The presenter also praised his team, adding: "I would like to give my warmest thanks and gratitude to everyone at Love Productions and Channel 4 and to Noelipops, Paul, Dame Prue, the crew and, of course, the wonderful bakers for welcoming me into the tent.
"I wish whoever takes over all the very best and I can't wait to tune into the next series without already knowing who won! xxx Matt".
His co-host Fielding admitted he would miss Lucas' "spark in the tent" as he paid tribute to him in a lengthy comment under his Instagram post.
Fielding wrote: "Totally respect your decision matt! But I will miss your spark in the tent and I will miss you channelling other characters at the drop of a hat like your brilliant Boris Johnson.
"I will miss your big smile and your sense of fun and silliness. I will miss our writing days in that ridiculous room with the high ceilings and I will miss us giggling like naughty school boys when Paul says "Eggy" in his Scouse accent.
"You were so lovely to work with and so kind to the bakers. Have fun on your next adventure and remember "It's all about the show stopper x x x"
"Was a pleasure for me to work with such a wonderful comic talent and a lovely man to boot xx Look forward to your next adventures as a friend and a fan x".
Judge Paul Hollywood also wrote on Twitter: "You will be missed @RealMattLucas, good luck with everything you've got planned ... you've been awesome xx."
While fellow judge Dame Prue Leith tweeted: "I have absolutely loved working with you @RealMattLucas.
"Thank you for bringing so much laughter and fun to the tent. x"
Bake Off's official Twitter account also reshared Lucas' statement and said it had been a "pleasure" to work with the comedian.
"We've loved having Matt Lucas brighten up our Tent for the last three years, especially when laughter and smiles were so much in need", the statement said.
"We appreciate everything he's done for Bake Off, from working in covid bubbles to supporting the bakers. It's been a pleasure - thanks Matt."
Following Bake Off's move to Channel 4 from the BBC in 2017, Fielding and Sandi Toksvig took over as presenters from Sue Perkins and Mel Giedroyc.
Toksvig announced her departure from the show in 2020 and was later replaced by Lucas.
Lucas and Fielding have been paired together for the past three series alongside Hollywood and Dame Prue as the show's judges.