Speaking at the Munich Security Conference in Germany, Biden said the conflict in Ukraine had moved beyond the need for a "reset" with the relationship, instead requiring a "re- assertion" of the "fundamental bedrock principles on which European freedom and stability rest."
Biden's blunt comments come at a time of increasing violence in Ukraine, with at least 224 killed and more than 540 injured in the final three weeks of January, according to the UN High Commissioner for Human Rights.
Biden yesterday said the United States was not trying to "collapse or weaken the Russian economy" with continued sanctions, but he had a warning for the Russian leader.
Western countries accuse Russia of arming the rebels and sending troops to Ukraine - claims Russia denies.
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Biden met with German Chancellor Angela Merkel and Ukrainian President Petro Poroshenko yesterday to discuss the situation in Ukraine.
"We must judge ... Any future agreement with Russia by the actions Russia takes on the ground, not by the paper they sign," Biden was quoted as saying by CNN.
"Given Russia's recent history, we need to judge it by its deeds, not its words. Don't tell us, show us, President Putin. Too many times President Putin has promised peace and delivered tanks, troops, and weapons."
"We will continue providing Ukraine with security assistance, not to encourage war, but to allow Ukraine to defend itself," he said. "Let me be clear: We do not believe that there is a military solution in Ukraine. Let me be equally clear: We do not believe Russia has the right to do what they're doing.