The 29-year-old Italian announced the decision via Instagram, just three months after beginning their partnership in April.
"We had some great results together, especially in Rome and Paris, and I will always remember those moments," Paolini wrote on the social media platform.
"I appreciate all the hard work and energy Marc gave every day.
"Now that this part of the season is over, I've decided to make a change. I've learned a lot and made good progress, and now I'm taking the time to reflect on what the next step will be. Thank you again, Marc, for everything. I wish you all the best in the future."
The coaching change marks another shift in a turbulent year for Paolini, who also ended a decade-long collaboration with former coach Renzo Furlan in March.
Currently ranked No. 5 in the WTA singles rankings - one spot below her career-high of No. 4 reached last October - Paolini is still chasing her elusive first Grand Slam title.
A two-time finalist, she fell to Iga Swiatek at the 2024 French Open and was beaten by Barbora Krejcikova in last year's Wimbledon final.
Her 2025 Wimbledon campaign ended in disappointment with a 4-6, 6-4, 6-4 loss to world No. 80 Kamilla Rakhimova in the second round.
Paolini had opened with a laboured 2-6, 6-3, 6-3 victory over Latvian qualifier Anastasija Sevastova, ranked No. 402. She was also eliminated from the doubles tournament on Friday at the All England Club.
Rakhimova went on to lose in the third round to No. 27 seed Linda Noskova of the Czech Republic, who was then defeated in the fourth round by American No. 12 Amanda Anisimova.
Anisimova is set to face No. 50 Anastasia Pavlyuchenkova of Russia in the quarter-finals on Tuesday.