Zverev opened the match with three straight aces and won 20 of his 21 service points in the first set in Sunday's clash at the Foro Italico.
The German didn't drop a point on his first serve until late in the second set when the 2.01m Jarry ran down a well-placed drop shot and replied with a cross-court winner.
In all, Zverev won 44 of his 49 service points — helped by getting in 95 per cent of his first serves.
It's been a long road to recovery for the world No.5 Zverev after tearing three ligaments in his right ankle during the 2022 French Open semi-final against Rafael Nadal.
When Zverev broke Jarry to convert his fourth match point, he dropped to his knees on the red clay, leaned back and let out a scream.
"The last two years have been extremely difficult," Zverev said during the trophy ceremony. "I didn't know whether I was ever going to be on this stage — regardless of winning or losing — so this moment is extremely special."
This year's French Open starts next Sunday and now Zverev has established himself among the favourites again — especially with world No.1 Novak Djokovic and 14-time Roland Garros champion Nadal both struggling lately.
Djokovic and Nadal were eliminated in the second and third rounds, respectively, in Rome.
There are also injury concerns for second-ranked Jannik Sinner (hip) and third-ranked Carlos Alcaraz (right forearm), who both withdrew from Rome.
"The focus is on Paris," Zverev said. "But let me enjoy this one for a day or so, and then I'll have my full focus on Paris."
But Zverev, who has disputed a penalty order from a German court over allegations that he caused bodily harm to a woman, faces a trial starting during Roland Garros. He said recently that he won't attend the start of the legal proceedings.
And he says he isn't 100 per cent healthy either. He had the pinky on his left hand bandaged due to a fall in his quarter-final win over Taylor Fritz, after which he said he "tore a capsule" and that his finger was "crooked." The German plays right-handed but uses a two-handed backhand.
Zverev will also be defending his gold medal when the Paris Olympics tennis tournament is held at Roland Garros starting in late July in what shapes as an exciting period for the German.