PARIS—French authorities said they have detained four more people in connection to the Louvre heist, including a man suspected of being the only thief to remain at large after purloining the nation’s crown jewels.

Paris Prosecutor Laure Beccuau said two men, ages 38 and 39, and two women, 31 and 40, have been taken into custody for questioning. Beccuau said all four detainees came from the Paris region, without disclosing further details.

Police said they suspected one of the men was part of the team of thieves who used a truck-mounted lift last month to break into an upper gallery of the world’s most-visited museum in broad daylight. He was detained in the town of Laval, in western France, though he is from Aubervilliers, the Paris suburb that was home to the other suspected thieves.

Tuesday’s arrests mean investigators believe they have tracked down the entire crew of thieves, having already detained three suspects in the aftermath of the robbery. Prosecutors brought preliminary charges against the three for criminal conspiracy and organized theft. A woman was also arrested on charges of complicity in organized theft and criminal conspiracy.

Investigators have given no sign they are any closer to finding the jewels. Authorities fear the jewels risk being broken down and sold off. The longer the jewels are missing, experts say, the less likely they are to be recovered.

The thieves made off with eight pieces of jewelry from France’s royal and Napoleonic-era collections valued at 88 million euros, equivalent to around $101 million, though French officials say that sum doesn’t capture the jewels’ historical value to France. Thousands of diamonds studded the jewels, as well as sapphires and emeralds the size of lozenges.

The heist shocked France and turned a spotlight on the porous security system of the Louvre and other museums across the country that have become the target of an increasing number of robberies.

The thieves parked the truck-mounted lift in a blind spot of the Louvre’s aging surveillance-camera system. They then used angle grinders to cut through a balcony window as well as the display cases that held the jewels in an operation that lasted just a few minutes.