Responding police officers closed the park to pedestrians for hours to search for the weapon until it was located.
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Authorities say the injured man was found on the southwest corner of the park just after 5:15 a.m.
He had sustained a gunshot wound to his leg and was taken to Bellevue Hospital with a non life-threatening injury.
Investigators say an unspent round was discovered in his pocket, and police immediately suspected the wound was self-inflicted.
Surveillance video later recovered by police reportedly showed the man accidentally shooting himself while sitting on a park bench.
The man is seen throwing the gun away as he walked to the intersection of Washington Square South and MacDougal Street, where he was discovered following a 911 call.
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Police officers canvassed the park until they found the gun.
The man is said to have an extensive criminal history, including arrests for drug dealing and possession.
NewsCopter 7 was above the crime scene Friday morning:
Man found shot in Washington Square Park