The gang of four Greek nationals and two Iraqis were arrested in Messolonghi, western Greece, on Wednesday as a small Piper plane carrying the migrants, including four children, was about to take off.
The migrants had been driven from Athens by the two Iraqi smugglers.
"A criminal network was dismantled for illegally transferring the migrants from Greece to countries in western Europe on small aircraft," the police said in a statement.
The network had successfully sent 12 groups of migrants to Italy, the police said, adding that each passenger paid the smugglers between €4,500 to €7,500.
The migrant children were sent to a juvenile welfare centre, police said. It was not clear what happened to the adults.
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Police also seized the Piper aircraft, €34,430 in cash, two cars, 700 grams of cannabis and shotgun cartridges during the raid.
The police identified the leader of the gang as one of the arrested Iraqis, and said they were continuing their investigation to find other accomplices.