The 55-year-old Spaniard, who took up the head coach's job in July 2016 for a two-year tenure, cited personal reasons for not renewing the contract which runs till the end of this season.
"Bengaluru FC and more importantly Indian football will always be grateful for the path that Albert Roca has shown us. Even in difficult situations he stayed true to his philosophy and brand of football and that is a testament to the manager and person he is," club CEO Parth Jindal said in a statement.
The next round -- inter-zonal play-off semifinals -- of the AFC Cup will be played in August.
Roca's impressive two-year spell saw Bengaluru become the first Indian club to make the final of AFC Cup in 2016.
His success was also highlighted by the Federation Cup (2017) and Super Cup (2018) titles that the club won to maintain the record of winning a trophy every season since its inception in 2013.
"His idea of how the game is to be played is what we need to be able to compete in Asia and on the world stage. He will always have a place at Bengaluru FC and we wish him the best for his future," Jindal said.
Roca, a former Barcelona FC assistant coach who arrived in the country at the start of 2016-17 season, left a lasting impression on Indian football with his philosophy of possession-based and free-flowing game.
Roca said though short, his stint at Bengaluru FC would always remain a special story in his career.
"It was one of the toughest decisions I have had to make in my managerial career but it's the right one. Bengaluru FC has been an experience I will always carry with me, no matter where I go," he said.
"The owners, the management, my staff, players and most importantly, the fans walked with me every step of this journey and I can never forget the love and support I have received here. I will miss being on the touchline for this club, but will always follow its progress."
Roca's first assignment for Bengaluru FC was the knock-out stages in the AFC Cup in 2016 and he went on to steer the 'Blues' all the way to final in Qatar where they went down 0-1 to Iraq's Air Force Club.
He put behind a disappointing fourth-place finish in the I-League to beat arch-rivals Mohun Bagan and win the Federation Cup.
Forced to rebuild the squad completely at the start of the 2017-18 season due to the Indian Super League draft, Roca got down to business and Bengaluru became the first Indian side to reach back-to-back semifinals at the continental stage.
After falling short against Tajikistan side FC Istiklol in the Inter-zone final in the 2017 AFC Cup, the 'Blues' arrived in the expanded ISL and finished the league stage in pole position with a record tally of 40 points from 13 wins and made their way into the grand final in their first attempt.
He helped BFC put aside the heartbreak of losing the ISL final against Chennaiyin FC in March, spurring them on to a triumphant Super Cup campaign last month.
In his two seasons in Bengaluru, Roca managed a staggering 60 per cent win percentage while achieving a record 15-match unbeaten run for the club early this year.
(This story has not been edited by Business Standard staff and is auto-generated from a syndicated feed.)