A Sydney father pointed a high-calibre pistol at his four-year-old daughter and pulled the trigger before letting her play with the gun, police have alleged.

Detectives have charged the 32-year-old man from the southern Sydney suburb of Revesby over the alleged incident as well as an illegal firearms cache and the production and possession of child abuse material.

He was charged with six offences by officers from Strike Force Bowser which is a NSW Terrorism Investigation Squad, however police said the investigation was not terrorism related.

Police said they seized a 25-calibre Walther TP-model pistol, two Colt 1911 45-calibre pistols and a Bentley-brand 12-gauge shotgun from premises at Revesby and Granville.

A Colt 1911-model pistol NSW Police say was seized as part of an operation in Revesby and Granville.

During the investigation, police said they also accessed mobile phone video footage which allegedly showed the man skylarking with one of the Colt .45 handguns, pointing it at his young daughter and pulling the trigger.

Officers said the weapon did not discharge.

The images also allegedly showed the man pointing the shotgun at the phone camera.

Detectives said further footage showed the child playing with the automatic pistol and pulling the trigger, without effect.

Senior police have condemned the alleged behaviour.

"Allowing a child to play with a firearm of any kind is reprehensible and is a serious criminal offence," Assistant Commissioner Mark Murdoch said.

The father has been remanded in custody and ordered to appear in Burwood Local Court on August 16.