Felix Herrera Garcia was allegedly seen in surveillance images running out of the day care with heavy shopping bags as the children were suffering from fentanyl exposure.
He was arrested Tuesday after the DEA tracked him to Sinaloa, Mexico, after a manhunt that lasted more than a week.
His wife and cousin are in custody and a third person, Renny Antonio Parra Paredes, was also arrested in the case. Prosecutors say he is a known drug dealer.
Federal authorities last week have promised to hold accountable anyone linked to the Morris Avenue day care.
New York City detectives were executing a search warrant on the Bronx apartment last week when they found narcotics, including a large quantity of fentanyl, and other paraphernalia concealed by plywood and tile flooring.
Photos shared by police show bags full of powder inside the "trap floor," a few steps away from a shelf of children's toys.
That grim discovery came nearly a week after four young children attending the day care in the Bronx apartment were treated for opioid poisoning. One of the victims, 1-year-old Nicholas Dominici, is believed to have died from the exposure.
The day care center operator, Grei Mendez, and a tenant of the building, Carlisto Acevedo Brito, were charged with murder of "depraved indifference" in Dominici's death.
Prior to finding drugs beneath the trap door, police had already announced the discovery of a kilogram of fentanyl that was stored near mats that children used for sleeping, along with multiple devices used by traffickers for mixing drugs and pressing it into bricks.
(The Associated Press contributed to this report.)
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Bronx day care death: Investigators find trap door in search for drugs
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