The shooting happened around 5:30 p.m. in the 5100 block of Archers Road.
When officers arrived, they found 5-year-old Cannon Hinnant suffering from a gunshot wound. Officers and EMS immediately began performing lifesaving efforts.
Hinnant was taken to Wilson Medical Center where the child later died.
Wilson Police identified the alleged shooter as Darius N. Sessoms, 25, of Wilson.
Police announced just after 4:30 p.m. on Monday that he had been arrested and was in the custody of Wilson Police Department officers and members of the US Marshals' Carolinas Regional Fugitive Task Force.
Charlene Walburn, a neighbor of Cannon, had a smile on her face when she described the little boy.
"He would come over, him and my husband would always talk back and forth and he would ask my husband to put air in his tire," she said. "If he saw me on the porch with a popsicle, he would always come over and ask me if he could have a popsicle."
But what happened Sunday night shocked them so much that they can't talk about it without choking up.
"We were eating our dinner and heard a bang. We knew it was a gunshot. So I told him to call 911, and I ran to the door."
They said they heard the cries of Cannon's father saying his son was shot.
"Our neighbor saw it. She said the young man just walked up to the little boy who was sitting on his bike, which he does every day."
"I just don't understand why he did it. How can you walk up to a little boy, point blank, and put a gun to his head and just shoot him? How could anyone do that?"