The former Blues boss is expected to end his time in Spain with Real Madrid this summer and said following the club's Champions League exit that he might not return next season, stating that he wants to go where he "feels loved".
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Villas-Boas told reporters: "He obviously wants to come back to England, whether he has a club aligned or not, we never know.
"It's extremely unlikely when someone makes it that public that something is not set out already but he is a great addition to the Premier League. He has a wonderful history in this league and I think it will be spectacular to have him back."
The current Spurs boss worked under Mourinho during the 50-year-old’s time at Porto, Chelsea and Inter, and believes his former boss' failure to win the Champions League in Madrid will be seen as an underachievement.
"When he left [England] he wasn't that well loved by a few of you guys [the media] and that was something we talked about.
"He was loved in all the clubs where he has won titles, in Real Madrid the same.
"There is maximum respect for what he has achieved, but for it to be at the level of Real Madrid's expectancy, we will never know. Probably not, but he certainly has won a league against a dream Barcelona team, which is a great achievement."