Peter Manfredonia, a University of Connecticut senior, is suspected of killing Ted DeMers, 62, and Nicholas Eisele, 23, before forcing Eisele's girlfriend into her car and fleeing the state with her.
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The woman, 23, was located Sunday at a rest stop near Paterson, New Jersey, with her 2016 Volkswagen Jetta, police said, and was not hurt.
Manfredonia, who is believed to be armed with several guns stolen during a home invasion, was last seen Sunday wearing a white T-shirt, dark shorts and carrying a large duffel bag near train tracks in East Stroudsburg, Pennsylvania.
Paterson is about a 90-minute drive from Derby, Connecticut, where Eisele was killed. East Stroudsburg is about an hour farther west on Interstate 80.
A lawyer for Manfredonia's family, Mike Dolan, said the suspect has struggled with mental health issues and has "sought the help of a number of therapists."
"Peter, if you are listening, you are loved," Dolan said at a news conference Monday. "It is time to let the healing process begin. It's time to surrender. You have your parents' and your sisters' and your family's entire support. So, Peter, from your parents, we love you, please turn yourself in."
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Connecticut State Police plan to hold a press conference Tuesday.
Manfredonia, a finance and mechanical engineering major from Sandy Hook, is suspected of killing DeMers and assaulting another man, possibly with a sword or machete, in Willington on Friday after they found Manfredonia walking along a road and offered him a ride back to his motorcycle.
The second victim, Nicholas Eisele, was found dead at his home Sunday in Derby, which is about 60 miles (96 kilometers) southwest of Willington and just west of New Haven. Eisele, a 2016 Newtown High School graduate, worked with his father in a landscaping and irrigation business. State police described him as an acquaintance of Manfredonia's.
Earlier on Sunday, a Willington man reported being held against his will by Manfredonia, who then left with food, several guns and the man's truck, which was later found abandoned near Osbornedale State Park, about a mile from Eisele's home.
Eisele's family set up an online fundraiser to help cover funeral expenses and far exceeded the goal of $10,000 in just a few hours. On the page, friends and family shared memories, including his love of his mother's German shepherds, Trooper and Sandy.