Mourinho has been linked with a return to Chelsea at the end of the season, and after the Portuguese coach hinted at his departure from the Bernabeu earlier this week, Villas-Boas has admitted that his arrival at Stamford Bridge would be "spectacular".
The 35-year-old 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."
Villas-Boas was part of Mourinho's backroom staff when he first arrived at Chelsea in 2004.