Aljofree, 21, joined United at the age of seven and progressed through every level of the club's youth system before making his senior professional debut.
He captained the Under-21 side this season, making 15 appearances in Premier League 2, and spent the first half of the campaign on loan at Notts County in League Two, where he made 11 appearances. The previous season saw him make 27 appearances at Accrington Stanley, scoring three goals.
He confirmed the news on Instagram.
"After 14 years at this amazing football club, my second home, and the place I've grown from a boy to man, I can't thank the staff, players and everybody who has helped me enough. I've made brothers for life and I will always appreciate what this club have given me. I wish everybody at the club the absolute best. Once a red, always a red."
Kobbie Mainoo, one of Manchester United's first-team regulars who also came through the academy, was among those to pay tribute publicly.
Sharpe, 20, has also confirmed his exit after five seasons at Carrington. The winger was considered one of the academy's more promising attacking prospects and featured in first-team training sessions during his time at the club.
Recurring injuries disrupted his development and he managed eight Premier League 2 appearances this season, registering one assist. He spent time on trial at Burnley earlier this year, featuring in one Under-21 fixture.
His farewell message read: "After 5 years my time at Manchester United has come to an end. I want to say thank you to the coaches, players, staff and the fans for my incredible time with this amazing club. Though my time had been difficult with injuries, I vow to do my best on the next part of my journey. Once a red, always a red."
Both players leave as free agents and will look to find senior football in the lower divisions of the Football League.