San Juan County Sheriff Bill Cumming said someone tried to break into an Ace Hardware store on the island at about 5:30 a.m. Sunday, and investigators believe it may be the work of Harris-Moore.
The break-in triggered an alarm siren, which apparently spooked the burglar into fleeing the scene.
Deputies immediately responded to the blaring siren and found that the building had been entered from the roof area. A window was broken - but nothing was taken and the intruder was nowhere to be found.
A manhunt was launched, as law enforcement officials scrambled to the scene with multiple units. Search dogs and a police helicopter were called in soon after from Whatcom County to assist with the manhunt.
"Investigators believe the initial scene evidence suggests Colton Harris-Moore to be the prime person of interest," Cumming said.
Several witnesses reported an unusual level of police activity across the island for several hours, including SWAT teams and search teams with dogs.
"Oh my God, it was like something out of a movie," said island resident Donna McCoy.
But search teams were unsuccessful in finding the suspect.
An investigator dusts for fingerprints at the scene of the break-in at the Orcas Island Ace Hardware store.
The evidence will be analyzed and then a final determination will be made of who is the prime suspect, Cumming said.
Harris-Moore, 18, has a long history of burglarizing homes in Washington state and Canada, only to disappear into the woods without a trace.
He has garnered considerable media attention and was nicknamed the "Barefoot Bandit" after allegedly committing some break-ins without wearing shoes.
Since he escaped from a halfway house in April 2008, Harris-Moore has been sought in scores of break-ins around Western Washington and is suspected of stealing four small planes and crashing each one.
Police suspect he's also stolen boats and luxury cars, and broken into dozens of homes and businesses, including several on Orcas Island during a previous crime spree there. His total haul may top $1.5 million, officials say.
It's believed Harris-Moore may have returned to Orcas Island on Feb. 10, when a stolen plane landed on the island after dark and a local grocery store was broken into and burgarized.
Many residents say they just want the teenager caught, before things get even more serious.
"He hasn't hurt anybody yet, but I think he's very capable of hurting someone - and I think there's been so many places being watched - the boats, the marinas - he's probably stuck here now," says McCoy.
A lot of people on the island know that he could be anywhere.
"What I'm nervous about is that there are so many places for him to hide," said Denise O'Toole. "He could be under a porch, he could be in a house that's unoccupied, he could be out in the woods. There are so many places for him to hide and lay low."
Island resident Darrel Suthergreen agreed.
"Yeah, it's disconcerting," he said. "A lot of people have lost a lot of property damage and cash. It hurts them. I think most of the people think - that's enough."