The actions come on the heels of Sunday's referendum in Crimea, in which nearly 97 per cent of voters supported breaking away from Ukraine to join Russia. Crimea's parliament swiftly declared the region an independent state.
Canada, along with the 28-nation European Union and the United States, doesn't recognize the outcome of the vote and says the referendum was illegitimate and unconstitutional.
"The so-called referendum held today was conducted with Crimea under illegal military occupation," Harper said in a written statement on Sunday. "Its results are a reflection of nothing more than Russian military control.
"Mr. Putin's reckless and unilateral actions will lead only to Russia's further economic and political isolation from the international community."
Earlier, the EU and the United States announced travel bans and asset freezes on 21 high-ranking Russian and Ukrainian officials linked to pushing the strategic Crimean peninsula to secede from Ukraine. The names of those individuals have not yet been released.
The Canadian government has already frozen the assets of 18 Ukrainian officials from the Yanukovych regime, as well as announced travel bans against individuals deemed responsible for threatening Ukraine's territorial integrity.
Harper will be travelling to Ukraine on March 22 to meet with acting Ukrainian prime minister Arseniy Yatsenyuk, en route to the Nuclear Security Summit in The Hague, Netherlands.