"I'll get to the point right away," Brady, 45, said in a video posted to Twitter Wednesday.
"I'm retiring for good. I know the process was a pretty big deal last time, so when I woke up this morning, I figured I'd just press record and let you guys know first.
"It won't be long-winded. You only get one super-emotional retirement essay, and I used mine up last year."
The seven-time Super Bowl champion also thanked his family, friends, teammates and competitors for their support during his illustrious career.
"Thank you guys for allowing me to live my absolute dream," he said in the short video. "I wouldn't change a thing."
Brady had initially retired in February 2022, but the decision proved temporary as he returned for one more season with the Tampa Bay Buccaneers.
He is considered by many to be the greatest quarterback of all time, having led the New England Patriots to six Lombardi Trophies and the Bucs to one.
During his long career, the three-time league MVP has broken almost every passing record, including regular season passing yards (89,214) and passing touchdowns (649). He has also amassed the most wins of any player in NFL history (251).
"The greatest ever," the NFL tweeted on Wednesday.
Some members of the Tampa Bay Buccaneers organization were informed around 6 a.m. ET Wednesday of Brady's decision to retire, a team spokesperson told CNN.
After Brady made his decision public, Buccaneers General Manager Jason Licht said the quarterback's legacy was "unmatched in the history of this game."
"All the Super Bowl titles and statistical records speak for themselves, but the impact he had on so many people through the years is what I appreciate the most," Licht said in a statement.
"His imprint on this organization helped take us to the mountaintop. We will certainly miss him as our quarterback, but I will also miss him as a leader and friend.
"Our entire organization is indebted to him for what he provided us over the past three years. We won't ever forget the wins or the accolades and his influence will be felt for years to come."
Selected 199th overall in the sixth round of the 2000 NFL draft by the Patriots, Brady played 20 seasons in Foxborough.
He left New England as a free agent after the 2020 season and signed with the Bucs where he led the team to a Super Bowl win in 2021.
A shoo-in for the Pro Football Hall of Fame, Brady will be eligible for election in 2028 when fans will get the chance to celebrate his incredible career all over again.
"Greatest of All Time. No question, no debate. It's been an honor and a privilege," JJ Watt -- one of the best defensive players of all time -- tweeted Wednesday.
He added: "The newly retired group meets on the golf course every morning at 10am. Drinks are on the new guy, so bring your wallet."
Despite all his success, Brady found winning a lot tougher during his final season in the NFL.
The Bucs finished with an 8-9 record, with many of their stars not performing at the level which helped them win a title two seasons ago.
Brady, who was due to be a free agent in the offseason, didn't look like his unflappable self either, with unusual errors and uncharacteristic mistimings creeping into the Tampa Bay offense.
It was also a difficult year off the field, with Brady going through a divorce from his wife of 13 years, Gisele Bundchen.
Despite the difficult final year of his career, Brady marches off into the sunset as the owner of more Super Bowls than any individual NFL franchise, a 15-time Pro Bowler and a strong case as, not just the greatest NFL player of all time, but one of the best athletes ever in any sport.
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