The victims were struck when gunfire erupted on 10th Avenue at West 207th Street just after 11:40 p.m.
James Michael, 44, was shot in the face and pronounced dead at Harlem Hospital.
Alejandro Ramirez, 40, was shot in the chest and pronounced dead at NewYork-Presbyterian Allen Hospital.
Police believe those killed may have been targeted.
A third man, 37, was shot in the leg and taken to Harlem Hospital in stable condition. Police do not think he was involved.
The suspect, a man wearing all black and a black mask, fled on foot eastbound on West 206th Street.
No arrests have been made and the motive for the gunfire is unknown.
The shooting occurred near the steps of the 207th Street subway station.
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