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
Goal exclusively revealed last September that Spurs and pinpointed the former England No.2 to head a restructure of their recruitment operations before stepping up their interest in May with a director of football position lined up.
Spurs chairman Daniel Levy is keen to reintroduce a continental-style set-up to aid manager Andre Villas-Boas five years after abandoning a similar model when Damien Comolli was sacked in October 2008, and 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 backfired; namely former manager Luis Enrique and players Fernando Gago and Jose Angel all leaving the Olimpico Stadium.
Tottenham, though, are keen to crank up their 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.