Daquan Breland, 23, and Daquan Wright, 19, were taken into custody about 6 a.m. Friday at an apartment complex in Wilkes-Barre, said Martin Pane, U.S. marshal for the Middle District of Pennsylvania.
Authorities had been seeking the New York City men for questioning in Sunday's death of 1-year-old Antiq Hennis in Brooklyn.
Authorities say the boy's father was pushing him in a stroller while crossing a street in the Brownsville neighborhood of Brooklyn on Sunday evening when multiple shots were fired. The child was struck on the left side of his face and later pronounced dead at a hospital.
Police believe the child's father, Anthony Hennis, 21, was the intended target, and the gunfire may have been gang-related.
Hennis had just picked up Antiq at the home of the baby's mother, Cherise Miller, to take him to visit Hennis' grandmother, police said. Hennis put the boy in the stroller and was pushing him across the street when four shots were fired, police said.
Mayor Michael Bloomberg called the killing "a tragedy for (the child's) family, for this community, for the entire city."
The killing was at least the second case of a toddler being shot to death in a stroller this year. In March, a woman walking home from a post office in Brunswick, Ga., with her 13-month-old son was accosted by a gunman who demanded her purse and then shot her in the leg and fired a shot at the child in his stroller, killing him, authorities said.