Clint Dempsey's second-half goal ultimately proved to be the matchwinner as Tottenham emerged from a second-half pummeling to secure a 3-2 victory at Manchester United.
It was the first time Spurs had won at United since 1989 and Villas-Boas said: "We wrote history for our team. The satisfaction comes from that.
"The players really felt they could nick a win here and the overall performance was an expression of that desire and ambition, though in different ways.
"In the first half, we attacked and kept the ball. In the second, we defended."
However, in the aftermath of such a momentous performance, Villas-Boas refused to talk of his team as potential league champions, something Spurs have not achieved since 1961.
"I don't think so," he said. "A couple of days ago, we were exactly the opposite.
"This is a very special night for us but our quest is to qualify for the Champions League.
"It is very difficult to go for the title. We understand it is a place where the great teams of this country belong.
"We want to win a trophy this season - and we want Champions League qualification."
Having expressed his hope during the game that his status as Tottenham's last matchwinner would be erased, Gary Lineker was delighted at the eventual outcome.
"Tottenham's season comes alive as an irksome stat of 23 years dies!" said the legendary sharpshooter on Twitter.
Victory was not achieved without a struggle, even after Jan Vertonghen and Gareth Bale had put Tottenham into a deserved lead at the break.
Fuming at his side's failure to match the speed and intensity of their opponents, Sir Alex Ferguson responded by introducing Wayne Rooney.
The response was immediate. Rooney crossed for Nani to halve the defecit, then Robin van Persie set up Shinji Kagawa to end a breathless spell of three goals in four minutes.
However, Dempsey's tap-in ensured the visitors still had their noses in front.
"At half-time we knew we weren't going to get out of Old Trafford without a fight," said Villas-Boas.
"Last season I was in charge of a Chelsea team that was 3-0 up against United and didn't win. That is an example of what they can do."
However, even though Bale had only trained once this week due to the effects of a virus, Tottenham's battling qualities came to the fore.
And after Van Persie had wasted an outstanding chance and both Rooney and Michael Carrick had struck the frame of Brad Friedel's goal, Spurs held on for a famous win.