They allegedly tailgated the vehicle before one of them climbed onto the bonnet of their van and broke into the truck in front of them.
Boxes of iPhones were then passed back through the van's roof.
The theft took place on the night of 24 July, on the A73 motorway near Horst.
Dutch news outlet ED said such gangs often modify their vehicles by putting an anti-slip mat on the bonnet.
The risky theft tactic was first seen in Germany in 2008, the outlet said. Belgium has witnessed similar incidents, almost all targeting smartphones. Sometimes, a grinding wheel is used to break into the truck.
Police spokesman Ed Kraszewski said Dutch police had been investigating truck thefts for some time, but doubted a theft like this could be pulled off.
"The truck was taking its freight from A to B and did not stop. Even so [the phones] were gone," he said. "So it must have happened that way. And now we finally have the evidence, with the van and the loot."
The men, aged from 33 to 43, were arrested on Saturday at a holiday park in Otterlo, in the central province of Gelderland.
Police found iPhones at the address, and the van they believe was used in the crime.
The men are set to appear before a judge on Tuesday.
Five Romanian men have been arrested in the Netherlands on suspicion of stealing iPhones worth 500,000 euros ($590,000; £447,430) from a moving truck.