The group stole $200,000 worth of Rolex watches during the heist in July of 2013.
The FBI says Allen Williams, Roberto Grant, Terrell Ratliff and Tyrone Dehoyos are also linked to three other high-end robberies, including one at a Cartier store in New York City last month.
According to federal court papers, Williams admitted to participating in the robberies. He allegedly cut himself on the display case during the Borgata heist, and a test on DNA recovered at the scene linked him and Ratliff to the robbery.
Furthermore, Williams allegedly admitted to driving Grant to the Cartier robbery.
The men are accused of taking more than $1 million in jewels over the course of their crime spree.
Dehoyos was arrested Tuesday in Brooklyn, New York. The other three were already in custody.
