The Argentine, now preparing to lead the United States at this summer's World Cup, spoke about Kane on the Stick to Football podcast, explaining how he inherited him as a third or fourth-choice striker under Tim Sherwood.
"When we started to work with Harry, we saw that his mindset was determined to be successful," Pochettino said.
"It's true he didn't have the best habits, but after we had a talk with him, he was very intelligent and was quick to change those habits — training, food, et cetera. We feel proud, but it's him and the people that are next to him that made him successful."
Kane went on to become Tottenham's all-time record scorer with 280 goals across all competitions, overtook Wayne Rooney as England's leading marksman, and has since plundered 54 goals in 46 appearances for Bayern Munich this season to help the German club win back-to-back Bundesliga titles.
Pochettino also left the door open to a future return to the Premier League, drawing a clear line between his coaching philosophy and the English game.
"I really love Tottenham. It's one of the most important parts of my life as a coach and in my personal life too. What I can tell you — for me it's one of the biggest clubs in the world."
He added that the Premier League remains a personal ambition.
"One day, yes, because I really like England. I think my human profile and coach profile match very well with the Premier League and with the culture, the idea, the idiosyncrasy, and the philosophy."
Tottenham have since appointed Roberto De Zerbi as head coach on a long-term contract, meaning any Pochettino return would have to wait.