The suspects are accused of armed robbery and grand auto theft.
An investigation is underway on whether the suspects are implicated in a string of recent home invasions in various upscale Athens neighbourhoods.
Two handguns, ammunition, burglary tools and masks were found in two residences.
According to reports, the 25-year-old was released from a prison in Grevena in December 2010 after serving a seven-year sentence for thefts and other crimes.
Meanwhile, in an unrelated development, a Georgian national was charged with no less than 73 break-ins of vehicles, mostly in southern coastal Athens.
The man, 28, had also been previously arrested but released on bail.