Ramos' contract, which is due to expire this summer, will not be renewed, making him available on a free transfer.
"Tomorrow is a special day, tomorrow I will say goodbye to another stage of my life, goodbye to @PSG_inside," Ramos posted on social media. "I don't know in how many places one can feel at home, but without a doubt PSG, the fans, and Paris were one of them for me.
"Thank you for two special years in which I was able play in every tournament and give my all. I will face new challenges, I will wear other colours, but first, and for the last time: ¡#AllezParis."
Added PSG chairman and CEO Nasser Al-Khelaifi in a statement: "We would like to express our immense gratitude to Sergio Ramos for the two years he has spent with us.
"Sergio's leadership, team spirit and professionalism, combined with his experience at the highest level, make him a true football legend, and it was an honour to have him in Paris. Everyone at the club wishes him all the best."
Ramos, 37, joined PSG in the summer of 2021 after spending 16 years at Real Madrid, during which he won five LaLiga titles and four Champions League crowns. A 2010 World Cup winner with Spain, the defender made 57 appearances and won Ligue 1 titles in both of his seasons at PSG but the club failed to make it past the round of 16 in the Champions League.
Following another season of disappointment in Europe, PSG are expected to undergo a significant transformation this offseason.
PSG manager Christophe Galtier confirmed on Thursday that Lionel Messi will also leave when his contract expires this summer, while sources have told ESPN that Neymar and PSG are both open to the Brazilian forward departing.
Ramos also announced his retirement from international duty in February after making 180 appearances for Spain. In addition to the World Cup, he won the European Championship in 2008 and 2012.
PSG, who clinched the Ligue 1 title last weekend, will play their final game of the season at home to Clermont Foot on Saturday.