After police started investigating activities at Sunshine Day Care in Goldsboro, they learned two more children had been sexually assaulted, they said.
DeMarlo Armstrong, 19, was charged with two more counts of first degree sex offense, authorities said.
The victims are girls, ages 4 and 6. Armstrong was placed in the Wayne County Jail under a $200,000 secure bond.
Wayne County sheriff's deputies initially arrested Armstrong on Nov. 7 and charged him with first-degree sexual offense and indecent liberties with a child. The child in that case is 4 years old.
Armstrong works at the Sunshine Day Care Center on 800 Lynch Drive in Goldsboro, which is owned by his mother.
Detectives urge any parents with children at the day care to call them with any concerns.
The Sunshine Day Care Center's license has also been suspended.
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