The Italian has parted company with the Serie A club despite having two years left to run on his contract at the Olimpico Stadium, with a move to White Hart Lane strongly mooted
Spurs chairman Daniel Levy is keen to reintroduce a continental-style setup to aid manager Andre Villas-Boas five years after abandoning a similar model when Damien Comolli was sacked in October 2008, and the looks close to confirming the new structure following the Italian's resignation.
"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 told the club's official website.
Roma president James Pallotta added: "We thank Franco Baldini for his service to AS Roma over the past two seasons. He played an important role in the launch of our project. We wish him well in his future endeavors."
Baldini had come under fire during last season following a number of decisions that have backfired, namely former manager Luis Enrique and players Fernando Gago and Jose Angel.
Tottenham, though, is keen to crank up its recruitment drive after again missing out on Champions League football on the final day of the season, with the likes of long-term target Leandro Damiao again on Levy's radar.