Zelenskiy met President Sergio Mattarella and then Prime Minister Giorgia Meloni before he was due to head to the Vatican for talks with Pope Francis, who said in late April the Holy See is involved in a peace mission to end the war with Russia.
Both Mattarella and Meloni reiterated Italy's full support for Ukraine in terms of military, financial, humanitarian and reconstruction aid in the short and long term.
At a news conference after her meeting with Zelenskiy, Meloni condemned Russia's "brutal and unjust aggression," pledged Italy's support for Ukraine for "as long as is necessary," and urged Russia to immediately withdraw.
"You can't achieve peace through a surrender," she said, echoing a previous comment by Mattarella. "It would be a very grave precedent for all nations of the world".
She emphasised Italy's support for Ukraine's membership of the European Union and the "intensification" of a partnership with NATO.
As he headed to the presidential palace, Zelenskiy's motorcade passed by small groups of people holding Ukrainian flags. One person held up a sign condemning Russia.
Zelenskiy flew to Rome on an Italian government plane that was escorted over Italian airspace by fighter jets. He was due to be received in Berlin on Sunday.
The meeting with the pope is expected to be the most significant part of Zelenskiy's time in Italy. He previously met the pope at the Vatican in 2020 and the two have had several phone conversations since the war began.
At the start of the war, the pope tried to take a balanced approach in hopes of being a mediator but later began forcefully condemning Russia's actions, comparing them to some of the worst crimes against Ukraine during the Soviet era.
Returning from a trip to Hungary on April 30, Francis made an intriguing but puzzling comment about the Vatican being involved in a mission to try to end the war. "There is a mission in course now but it is not yet public. When it is public, I will reveal it," he told reporters during his flight home.
Francis met this week with Russia's outgoing ambassador to the Vatican, Alexander Avdeyev, and the Italian newspaper Il Messaggero reported that the Vatican may have given the envoy a letter for Russian President Vladimir Putin.
Francis has pleaded for peace practically on a weekly basis, and has repeatedly expressed a wish to act as a broker between Kyiv and Moscow. His offer has so far failed to produce any breakthrough.
The pope has a standing invitation from Zelenskiy to visit Kyiv but the pope has said previously that he also wants to visit Moscow as part of the same peace mission.
Ukrainian Prime Minister Denys Shmyhal met the pope at the Vatican on April 27 and said he had discussed a "peace formula" put forward by Zelenskiy.
Zelenskiy and his team have been vigorously promoting Kyiv's 10-point peace plan and urging world leaders to hold a Global Peace Summit based on the proposals.
It calls for restoring Ukraine's territorial integrity, the withdrawal of Russian troops and cessation of hostilities, and the restoration of Ukraine's state borders. Zelenskiy has repeatedly said the plan is not open to negotiations.
The pope has said the Vatican is willing to do "all that is humanly possible" to help the repatriation of Ukrainian children. Kyiv estimates nearly 19,500 children have been taken to Russia or Russian-occupied Crimea since February 2022, in what it condemns as illegal deportations.
(Reporting by Philip PullellaAdditional reporting by Olena Harmash, Max Hunder, Gavin Jones and Giselda VagnoniEditing by Grant McCool, Frances Kerry and Helen Popper)
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