The Brit won six of his seven world titles under the tutelage of Wolff, but had fallen behind many of his rivals in recent years, prompting him to seek a change in scenery.
He will now join Charles Leclerc at the Scuderia, where he hopes to rediscover the kind of form which can put him in a position to challenge for a historic eighth championship crown.
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Wolff looks ahead to life after Hamilton
Wolff replaced the 105-time race winner with teenager Kimi Antonelli, who will make his F1 debut alongside George Russell at the season-opening Australian Grand Prix on March 16.
Having ended the previous campaign fourth in the constructors' standings - almost 200 points behind winners McLaren - the team is targeting major improvements.
Wolff has made no secret of the fact he was sorry to see Hamilton go, but is optimistic about what his new driver pairing can deliver going forward.
However, in an interview with Sky Sports, the Austrian has admitted that while Antonelli's arrival may generate much of the attention, he has been disappointed in the lack of recognition which has come the way of Russell in recent years.
"It was right for both of us," Wolff said as he reflected on Hamilton's exit.
"I think when you see Lewis in his first appearances at Ferrari, this picture in front of Enzo Ferrari's house, it's iconic. Lewis with his sense of style, and I've told him.
"And at the same time, us embarking on a different route, trying to reinvent ourselves with a young driver - in addition to George, who isn't mentioned enough.
"We have a senior, accomplished driver that has won races, and this new kid coming up.