The mother of one of the victims shared her story with ABC11 Tuesday - hoping it will help identify and catch the suspect.
Authorities says the incidents happened in the 4000 block of Deep Hollow Drive and the 2600 block of New Hope Church Road. One incident involved a 4-year-old boy who was flashed by the suspect. In the second, police say the man inappropriately touched a 3-year-old girl.
"He took off her skirt and touched her," said the child's mother - who ABC11 is not identifying. "He slapped her in the face and was telling her to shut up, grabbed her by the arm, and had her up in his arms and apparently she screamed until he let her go."
Other kids in the neighborhood heard the screams and ran inside to tell adults.
"We were running down the stairs and we saw the green truck take off," neighbor Ty Pyatt recalled.
Police say they're looking for a man in his twenties or thirties, who is either balding or has very short hair. The suspect has a small beard or goatee, tattoos on his arms - possibly one of a naked lady according to the victim - and he may have a tongue piercing.
Eyewitnesses say he was in a green Chevy or Dodge pickup truck.
After the incident off Friday, the little girl's mother says other kids told her the same guy had tried to lure them away.
"He's offered kids candy, kids money, he's offered - come with me to the ice cream truck," she said.
Raleigh police were back in the area Tuesday conducting more interviews.
The little girl's mother hopes an arrest comes soon - thinking about what else could've happened to her child and worrying about what might happen to someone else's.
"That could've been my little girl's life. He needs help. He needs to go. I hope they catch him, they got to. If it's not my little girl, he missed that one somebody else's is in danger too," she said.