According to surveillance video, the thief smashed through the glass door around 11:30 Sunday night and spent more than three hours inside.
The suspect took five flat-screen televisions. The suspect was seen on video stopping to grab a drink in a mini-fridge and picking through a pile of donated clothes.
Corps Officer David Repass walked an ABC11 crew through other parts of the building that were rummaged through, including a clothing and food storage closet room.
"They just pilfer through there, so they may have taken some things," said Repass.
A children's nursery was also ransacked.
Repass said old computer equipment was taken from a room and that something was rolling on one of the monitors that should have stopped the thief in his tracks.
"They walked by the monitors that showed they're being recorded. So, no idea how they didn't think, you know, wait a minute," said Repass.
The center is expected to reopen Tuesday.
The staff has been dealing with the cleanup and is also trying not to lose focus on the upcoming Back to School Giveaway on Aug. 24 from 10 a.m. to noon. The Salvation Army is still working to collect school supplies for those in need.
Repass only transferred to this Salvation Army six weeks ago.
He said he does feel compassion for whoever stole from this charity-based Christian institution.
"We're interested in helping people," said Repass. "I would say to anyone, if you were considering making a wrong decision, let us help you -- maybe point you in the right way, because that's what we're here for."
Durham Police says they're still working to gather suspect information.