Paul Gascoigne has quit his position as player-coach of Boston United after just over two months at York Street.
The 37-year-old former England midfielder plans to complete a coaching course at Lilleshall before trying to get a player-manager role.
"I've left on professional terms. I just think I needed to extend my career on the coaching side," Gascoigne said.
Boston boss Steve Evans said: "I would like to think we will work together again, sooner than people may imagine."
Pilgrims chairman Jon Sotnick added: "It is a sad day, but Paul feels he needs to fulfil his career aspirations."
Gascoigne, who counts Newcastle, Tottenham, Lazio and Rangers among his former clubs, earned 57 England caps and was one of the stars of the 1990 World Cup and Euro 1996.
He had a brief stint as a player-coach in China before a failed attempt at reviving his player career in England with Wolves.
After joining Boston, Gascoigne made five appearances, helping the club to ninth in League Two.
His last game for them was in the Carling Cup tie against Fulham three weeks ago, which the Pilgrims lost 4-1.
Evans added: "Paul has been an integral part of my management team and has played a key part in our recent success."
Gascoigne said: "I've shaken hands with the gaffer (Evans) and I've shaken hands with the chairman (Sotnick) and said bye-bye to the lads.
"I think it's one of the hardest decisions I've had to make in my professional career so far. I've done it for professional reasons."
Gascoigne will attend a Football Association course run by Sammy Lee, the former Liverpool midfielder who is now one of Sven-Goran Eriksson's England assistants.
"Sammy Lee has a coaching course coming up and I want to go and prove myself
as a coach, as I wanted to at the start of the season, and hopefully in the
future as a manager," said Gascoigne.
"I'll be speaking to Sammy tomorrow to see what's the way forward for Paul Gascoigne.
"The reason why I want to leave isn't about bad feelings with the club or any bad feelings with me, it's for professional reasons and I hope they understand that.
"I want to be a top coach and I'll be speaking to the top coaches around the country and learning a lot more about my badge and management.
"This is something I took up on my own shoulders. I think it's right for me, what I'm doing."
Gascoigne added that he is winning his battle against alcohol.
"I think Paul Gascoigne two years ago would have run away to a bottle of whisky. Now I don't do that," he said.