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With Ukraine reporting Russia has massed 45,000 troops on its border, NATO said there was a "high probability" that Moscow could intervene militarily in the country's east, where Kiev's forces are closing in on pro-Russian separatists, Reuters said.
Western countries believe that Russian President Vladimir Putin - who has whipped up the passions of Russians with a nationalist campaign in state-controlled media since annexing Crimea from Ukraine in March - could now send his forces into the east to head off a rebel defeat.
Itar Tass news agency said the convoy has departed from near Moscow which means it would take it a couple of days to arrive in east Ukraine, some 1,000 km (620 miles) to the southwest.
"It has all been agreed with Ukraine," Business FM radio quoted President Vladimir Putin's spokesman, Dmitry Peskov, as saying.
Thousands of people are believed to be short of water, electricity and medical aid due to the fighting. U.S. President Barack Obama said that any Russian intervention without Kiev's consent would be unacceptable and violate international law.
European Commission President Jose Manuel Barroso also warned on Monday "against any unilateral military actions in Ukraine, under any pretext, including humanitarian".
Russian state television Rossiya 24 showed several heavy white trucks departing from the town of Alabino near Moscow.
A Rossiya 24 correspondent at the scene said the convoy should arrive at the Ukrainian border in 2 to 3 days where it would meet a representatives of the International Committee of the Red Cross (ICRC).
Russia has said the aid would be delivered together with the ICRC.
The ICRC said on Monday it had submitted a document to Russian and Ukrainian officials.