Police in suburban Gwinnett County said Shembo was charged after his then-girlfriend's dog died from blunt force trauma last month.
The Falcons moved quickly to cut ties with the player.
"We are aware of the charges that have been filed against Prince Shembo," the team said in a statement. "We are extremely disappointed that one of our players is involved in something like this. Accordingly, we have decided to waive Prince Shembo."
The case was especially sensitive to a franchise that lost star quarterback Michael Vick after he was charged with running a dogfighting ring in 2007. Vick wound up serving federal prison time and never played again for the Falcons.
Denicia Williams called police on April 19 to report that her ex-boyfriend had killed her dog, police said in a news release. Williams told investigators she had taken her Yorkie, Dior, to Shembo's apartment on April 15.
At some point, she left the 6-foot-2, 254-pound Shembo alone with the dog, and when she found the dog later he was unresponsive.
Williams took the animal to an animal hospital where he died shortly afterward. Shembo told her over the phone the next day that he had kicked the dog, and she ended their relationship, Williams told police.
Shembo surrendered at the Gwinnett County jail Friday night and his bond was set at $16,700 according to county records. Attorney Jerry Froelich told reporters that Shembo said he was putting the dog in its cage and he kicked it after it bit his hand.
"When you're a small dog it doesn't take much with the size he is," Froelich said, adding that the dog's death was accidental.
Shembo, 23, was a fourth-round pick in 2014 out of Notre Dame. He got significant time at inside linebacker as a rookie, playing in all 16 games with three starts and making 59 tackles.
New coach Dan Quinn planned to move Shembo to outside linebacker and give him a shot at a regular role in the pass rush rotation.
Now, the Falcons will have to come up with another option.
A necropsy on the dog's body was done April 21 and tissue samples were sent to the University of Georgia for further testing. Police got the final results on Thursday.
While waiting for those results, a police investigator spoke to Shembo several times by phone. Police decided to take out a warrant for Shembo's arrest because of inconsistencies in his account of what happened and because of the necropsy results, the release said.
The dog suffered extensive injuries, including a fractured rib, abdominal hemorrhage, head trauma, eye injuries and extensive bruising in the muscles of his front leg and shoulders.
Police said an investigator contacted the Falcons to let them know about the warrant.
Froelich said he hadn't seen the police report as of Friday night.Suggest a correction