"If other measures do not work, then NATO should intervene like in Kosovo," Dzhemilev told AFP in a phone interview from Brussels, where he was preparing to meet NATO officials on Friday.
NATO intervention "usually only happens when there is a massacre, we want it to happen before there is a massacre," said Dzhemilev, currently a lawmaker in Kiev who spoke with Russian President Vladimir Putin in a phone call earlier this week.
Dzhemilev also criticised inaction in the West, saying: "We haven't seen any serious steps from the West. They imposed visa bans but so what? Those people (targeted by the bans) have a comfortable enough life in Russia."
Tatars are planning a series of demonstrations across Crimea today ahead of Sunday's vote under the slogan: "No to the illegal referendum!"
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"We are calling for the Crimean Tatars to boycott the referendum," Dzhemilev said.
Suspicion of Moscow is high among the Tatar community, who were the original population of the Crimean peninsula and were deported en masse by Stalin to Central Asia during World War II.
The Tatars only started returning home in the late 1980s and currently number around 12 percent of Crimea's mostly Russian-speaking population of two million people.
They have maintained their Turkic language and Sunni religion and Turkish Prime Minister Recep Tayyip Erdogan has also pledged his support.