The shooting happened at about 12:40 p.m. in the 500 block of North 16th Street in the city's Spring Garden section.
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The victims, ages 27 and 30, both died at the hospital after being shot in the face and the head, police said.
On Tuesday, officers executed a search warrant inside the alleged suspect's residence, but authorities say he was not there.
Chopper 6 was over the police response around 12:30 p.m. along the 500 block of North 18th Street.
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Police are not identifying the suspect at this time.
Anyone with any information is asked to call police at 215-686-TIPS.