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“I want everyone to hear me now, especially in Moscow. The time has come for a meeting, it is time to talk,” he said in a video address released in the early hours of Saturday.
“The time has come to restore territorial integrity and justice for Ukraine. Otherwise, Russia’s losses will be such that it will take you several generations to recover.”
The two sides have been involved in talks for weeks with no sign of a breakthrough.
Zelenskiy said Russian forces were deliberately blocking the supply of humanitarian supplies to cities under attack.
“This is a deliberate tactic … This is a war crime and they will answer for it, 100%,” he said.
Zelenskiy said there was no information about how many people had died after a theatre in the city of Mariupol, where hundreds of people had been sheltering, was struck on Wednesday. More than 130 people had been rescued so far, he said.
Rescuers in Ukraine searched on Friday for hundreds of civilians feared trapped under the wreckage of a bombed theatre, as local forces battled against Russian troops across the country.
President Volodymyr Zelensky said 130 people had been brought out after the Russian strike two days ago on the building where civilians were sheltering in the besieged city of Mariupol, but that hundreds were still inside.
With world powers manoeuvring to respond to the bloody three-week invasion, Washington said that President Joe Biden had told Chinese counterpart Xi Jinping of the “consequences” of any support for Russia.
The United States fears that China could deliver financial and military aid to Moscow, transforming an already explosive transatlantic standoff into a global confrontation.
In the nearly two-hour phone call, Xi said that war is “in no one’s interest”, but showed no sign of giving in to US pressure to join Western condemnation of Russia.
Russia’s offensive remains largely stalled, a US defence official said, with troops about 30 kilometres (20 miles) east of the capital Kyiv and facing heavy resistance.
The official added that Russian forces had made no further progress into the northeastern city of Kharkiv, which they have encircled, and that Ukrainians were also defending the northern city of Chernihiv.
Despite the apparent setbacks, President Vladimir Putin held a large triumphalist rally in a Moscow football stadium featuring a sea of Russian flags, pro-Kremlin pop stars and chants of “Russia! Russia! Russia!”
Marking eight years since Russia’s annexation of Crimea from Ukraine, tens of thousands of people took part, many wearing ribbons with the letter Z that features on Russian tanks invading Ukraine.
Putin said the Russian military was in Ukraine “to rid these people from their suffering and genocide”.
Also on Friday, the Russian leader accused Kyiv of “war crimes” in a call with French President Emmanuel Macron, and said that Moscow was doing “everything possible” to avoid civilian deaths — even as Russia continued its devastating bombardment of Mariupol and other cities.
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