The men have been identified as 50-year-old Frank Peterson III, and 40-year-old Anthony Johnson, both of Stamford.
The accident, which involved two cars, happened around 10 p.m. on Connecticut Avenue.
After extricating two males from the first car, firefighters pronounced both victims dead on scene.
The one male occupant who was in the second car was seriously injured and brought to Norwalk Hospital. His current condition is unknown.
Police say a preliminary investigation revealed that both cars were traveling in opposite directions and had a head-on type collision.
This accident remains under investigation. If you have any information to add to this investigation please call the Norwalk Police Department at (203) 854-3000.