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Le Pen has called for Macron to step down if his party suffers a major defeat in the election, arguing 'the only way out of a potential political crisis is for the president to resign'.
The first round on June 30 saw the largest gains ever for the anti-immigration, nationalist National Rally (NR), led by Le Pen.
Over 49million people are registered to vote in the elections, which will determine which party controls the 577-member National Assembly, France's influential lower house of parliament, and who will be prime minister.
If support is further eroded for Macron's weak centrist majority, he will be forced to share power with parties opposed to most of his pro-business, pro-European Union policies.
Voters at a Paris polling station were acutely aware of the the far-reaching consequences for France and beyond.
Racism and antisemitism have marred the electoral campaign, along with Russian cybercampaigns, and more than 50 candidates reported being physically attacked, highly unusual for France.
The government is deploying 30,000 police on voting day.
The heightened tensions come while France is celebrating a very special summer: Paris is about to host exceptionally ambitious Olympic Games, the national soccer team reached the semi-final of the Euro 2024 championship, and the Tour de France is racing around the country alongside the Olympic torch.
France's prime minister Gabriel Attal cast his ballot in the Paris suburb of Vanves on Sunday morning.
Macron voted later in the seaside town of Le Touquet.
Le Pen is not voting, because her district in northern France is not holding a second round after she won the seat outright last week.
Across France, 76 other candidates secured seats in the first round, including 39 from her NR and 32 from the leftist New Popular Front alliance.
Two candidates from Macron's centrists list also won their seats in the first round.
The elections wrap up on Sunday at 8pm in mainland France and on the island of Corsica. Initial polling projections are expected on Sunday night, with early official results expected late Sunday and early Monday.
Voters residing in the Americas and in France's overseas territories of Saint-Pierre-et-Miquelon, Saint-Barthelemy, Saint-Martin, Guadeloupe, Martinique, Guyana and French Polynesia voted on Saturday.
The elections could leave France with its first far-right government since the Nazi occupation in the Second World War if the NR wins an absolute majority and its 28-year-old leader Jordan Bardella becomes prime minister.
The party came out on top in the previous week's first-round voting, followed by a coalition of centrr-left, hard-left and Green parties, and Macron's centrist alliance.