Speaking at a press conference on foreign policy, the far-right presidential candidate said she would pull France out of the military command of the alliance.
She also proposed a “strategic rapprochement” between Russia and NATO.
Ms Le Pen said: “As soon as the Russian-Ukrainian war is over and has been settled by a peace treaty, I will call for the implementation of a strategic rapprochement between NATO and Russia.”
When discussing her policy on defence she added: “I would place our troops neither under an integrated NATO command nor under a future European command.”
Ms Le Pen is facing pressure to distance herself from her previous closeness to Vladimir Putin, having been accused of being “complacent” and “financially dependent” on Moscow by incumbent President Macron.
She has denounced claims of betraying French interests as being “inaccurate and particularly unjust”.
Ms Le Pen is currently polling at 45 percent, with President Macron the current frontrunner on 55 percent ahead of the final votes being cast on April 24.
Following her previous election defeat in 2017, Ms Le Pen was pictured shaking hands with Putin when he hosted her at the Kremlin.
At the time, she declared that she and Putin were part of a “new world order”, alongside then American President Donald Trump and said they shared “the same values”, reported The Guardian.
READ MORE: Putin humiliation as naval cruiser ‘seriously damaged’
President Macron has also faced criticism over his attempts to appease Putin with long phone conversations and an invite to the Palace of Versailles.
He has hit back at his political opponent for her nationalist stance, telling a rally in Strasbourg that “nationalism is war”.
The French President accused his rival of secretly pushing for “Frexit” as she knows the policy will not be popular in France.
Ms Le Pen said that she was no longer pursuing the idea of leaving the EU, but instead said she wanted to reform the bloc from within.