"Following discussions with ITV, Piers Morgan has decided now is the time to leave Good Morning Britain," ITV said in a short statement. "ITV has accepted this decision and has nothing further to add."
Earlier in the day, Morgan walked off the "Good Morning Britain" set after he was skewered by a co-host for his criticism of Prince Harry and Meghan following their blockbuster interview with Oprah Winfrey.
During the interview with Oprah, Meghan said she "didn't want to be alive anymore" and had contemplated suicide while pregnant with her son Archie. She said the royal family had told her she couldn't seek help because "it wouldn't be good for the institution."
On Monday's edition of "Good Morning Britain," Morgan questioned whether the Duchess was being truthful about having suicidal thoughts. His comments sparked a huge controversy in Britain, and he was rebuked by mental health charity Mind.
On Wednesday, Morgan said that he "still" does not believe Meghan.
"I've had time to reflect on this opinion, and I still don't [believe her]," Morgan tweeted. "If you did, OK. Freedom of speech is a hill I'm happy to die on. Thanks for all the love, and hate. I'm off to spend more time with my opinions."
UK media regulator Ofcom said it had received over 41,000 complaints about the program as of Tuesday afternoon. "We have launched an investigation into Monday's episode of Good Morning Britain under our harm and offense rules," it said in a statement on Twitter.
Morgan, who hosted a show on CNN from 2011 to 2014, faced criticism from his own colleague on Tuesday.
"I understand that you [Morgan] don't like Meghan Markle, you've made it so clear a number of times on this program," said "Good Morning Britain" co-host Alex Beresford. "And I understand that you've got a personal relationship with Meghan Markle, or had one and she cut you off," he added.
"Has she said anything about you since she cut you off? I don't think she has, but yet you continue to trash her," Beresford said.
At that point, Morgan got up and, while walking off the set, said, "Okay, I'm done with this, sorry, no, sorry... see you later, sorry, can't do this."
- CNN's Hanna Ziady and Stephanie Halasz contributed reporting.