Basil Shahin, 7, was listed in critical condition after the crash. He died Thursday, according to WakeMed officials.
His brother, Kaled Shahin, 9, also died.
The crash happened at about 4:45 p.m. Wednesday on the corner of Spring Forest and Falls of Neuse roads.
A woman and three children were attempting to cross Falls of Neuse Road, from east to west, when the boys separated from the mother and ran ahead.
The boys were struck by a 1992 Toyota 4 Runner traveling southbound on Falls of Neuse, said Jim Sughrue, spokesman for the Raleigh Police Department.
The third child also ran ahead but was not hit.
“The one thing I could say was, ‘Oh no! Oh no! Oh no!’” witness Sam Townsend said. “They just went flying up in the air and rolling on the pavement."
Police do not plan to file charges against the driver of the vehicle, 57-year-old Catherine Mary Biondi. The mother and children were traveling against the light, which was green for Falls of Neuse traffic, Sughrue said.
“The car coming had the green light and hit them,” witness Cheryl Barbour said.
The police have not released the name of the mother of the children. She did not file a witness report.