One of Andre Villas-Boas' main priorities this summer is to have a technical director in place by the start of next season. The Spurs boss feels he needs a bridge between the coaching staff and the board as was the case when he was at Porto and Inter Milan, where he worked under Jose Mourinho.
Baldini, who was assistant to Fabio Capello when the Italian was England manager, has been strongly linked with a move to White Hart Lane and his departure from Roma removes the biggest obstacle that prevented a switch to the north London club last season.
A Roma statement confirmed that they had "consensually ended the professional relationship" with Baldini, who was the club's general manager.
"I want to thank AS Roma's ownership for the opportunity to work together. I have enjoyed my time in Rome and wish the best to the club, the players and fans," Baldini said.
Ex-Spurs manager Martin Jol endured a fractious relationship with former director of football Damien Comolli, with the pair clashing over transfer targets.
Villas-Boas does not foresee any problems like that occurring again, though, should a technical director be appointed.
"It's not fundamental, but it will help the club moving forward," Villas-Boas said last month.
"It's something that I am used to working with. A number of experiences that we had with Jose (Mourinho) at Inter Milan with (Marco) Branca which was always positive.
"Not only me as a manager but when I was with him so I think it's something that works. Since the first day I told the club that it's somebody who is extremely important in my view to the structure of the club."