The coach also praised Gareth Bale for spurning offers from other clubs last summer to join the Blancos and lauded Pep Guardiola's legacy at Camp Nou
After honing his talent as Jose Mourinho's understudy, the Portuguese made a name for himself at Academica then Porto before struggling to inspire as Chelsea manager as he failed to survive his first season at Stamford Bridge.
He returned to the bench in the Premier League in charge of Tottenham but, after 18 months in the job, he was shown the door as Spurs' poor form showed no signs of improving in a troubled 2013-14 campaign.
Villas-Boas' failures in England have not put him off coaching top clubs, however, and he was not shy about suggesting he could be in charge of either the Catalans or the Blancos in the future.
"Real Madrid and Barca are two of the best clubs in the world," he told Marca. "One of them may have won more titles, but the other have made more of a mark in recent history - the legacy Pep Guardiola left is awe-inspiring.
"For me, as a young coach, it would be a dream to train either of them."
Villas-Boas coached Gareth Bale in his final season with Spurs before the winger joined Real Madrid for €100 million last summer and his former tutor praised the Welshman for following his ambition by joining the Spaniards.
"He's been amazing," the Portuguese coach added. "Although he scored many great goals in the Premier League last year so this is not a surprise.
"He has adapted very well at Madrid. He is aware that he is facing one of the biggest challenges of his career. Coming to the club was his decision, he had many offers but decided to go with the team with the most titles."