She is among the European politicians who have called for closer ties with Russian President Vladimir Putin.
"I am in favour of developing relations with Russia in the context of the long history that links our two countries," Le Pen said at the start of her meeting with Russia's parliamentary speaker Vyacheslav Volodin.
"I've pleaded at every level for cooperation between our countries in the fight against terrorism," she said, invoking Russia's role in Syria, where it has supported the regime of Bashar al-Assad, and France's role fighting Islamic extremists in Africa's Sahel region.
Le Pen did not have any planned meetings with Kremlin representatives or government officials during her Moscow visit.
The far-right leader has visited Moscow on several occasions, enjoying positive Russian state media coverage.
She is among the European politicians who have called for closer ties with Russian President Vladimir Putin and approved of Moscow's annexation of Crimea from Ukraine in 2014.
In 2014, the Front National received a nine-million-euro ($9.7 million) loan from a Russian commercial bank that later collapsed.
The party on Friday dismissed the possibility of seeking further funding from a Russian bank.
Moscow has been accused of seeking to promote anti-EU candidates, including populists, in European elections.
Last year, the Kremlin welcomed both the outcome of Britain's referendum on Brexit and the election of Donald Trump as US president.
Russian Foreign Minister Sergei Lavrov on Thursday said Le Pen was not a "populist" but a "realist or anti-globalist" figure.