State Police 1st Sgt. Dave Bursten said David Ludwig, 18, was apprehended about 12:30 p.m. EST after a car he was driving crashed about 20 miles west of Indianapolis following a pursuit by State Police.
"He's in custody and we have the girl," Bursten said.
Footage from news helicopters in Indiana showed a girl sitting in a police cruiser, and a young man wearing a gray T-shirt was handcuffed sitting next to a red Volkswagen Jetta that had run head-on into a tree on a curve of a rural road. The site is some 600 miles from the scene of the killings.
Authorities in Pennsylvania had said Ludwig had his parents' red Jetta.
The two had been spotted at a central Pennsylvania gas station Monday morning, but were not caught then.
The shift manager at a truck stop Subway shop in Lamar, about 90 miles from Borden's home, said she sold the couple an Italian sub at about 9 a.m. on Monday, and thought they matched a radio description she had heard earlier.
"Her face was all puffy, her eyes were puffy," Amanda Workman told The Associated Press. "You could tell she was crying."
Michael F. and Cathryn Lee Borden, both 50, were found shot to death at the family's home in Warwick Township, about 60 miles west of Philadelphia, shortly after 8 a.m. Sunday. The couple's 9-year-old son ran to the home of neighbors, who called 911, police said.
Workman said the young couple paid cash and had apparently made another purchase from a different part of the truck stop.
"They were really shady. They didn't want to talk a lot. They just ordered their sandwich and left," Workman said.