Officers found more than 900 violations and began making arrests Tuesday.
Besides illegal hunting, the violations include illegal use of dogs, operation of illegal bear enclosures and hunting on national forest lands without permits.
The four-year investigation targeted poachers mostly in the two states with some work in neighboring states.
Officers with the Georgia Department of Natural Resources and the North Carolina Wildlife Resources Commission infiltrated poaching circles to document violations.
“These arrests bring an immediate halt to those crimes and, we hope, will make would-be violators think twice before breaking the law,” said Col. Dale Caveny, law enforcement chief for the N.C. Wildlife Resources Commission.
Officials say it was one of the largest undercover wildlife operations in years.
Called Operation Something Bruin, the investigation also included the U.S. Forest Service, the U.S. Fish and Wildlife Service and the National Park Service.
“We all have a vested interest in safeguarding wildlife from poaching,” said Gordon Myers, executive director of the N.C. Wildlife Resources Commission. “By targeting wildlife thieves, Operation Something Bruin helps protect our outdoor heritage and conserves wildlife for future generations.”