An unattended fire left by squatters is believed to have ignited the blaze that gutted the former St John's boys home in Goulburn.
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More than a century of history went up in smoke on Wednesday afternoon as winds fanned the fire in the EC Manfred-designed building's second storey and roof cavity.
NSW Fire and Rescue Inspector Trent Lawrence said the investigation had been handed to Goulburn detectives, but arson had been ruled out.
"Once safe last night, our crews have been able to gain access to the second storey and investigate the damage," Inspector Lawrence said.
"At this stage, we're not putting the fire down as suspicious, but we believe a small fire was left unattended by squatters in the building."
The fire caused substantial damage to about 80 per cent the roof with "some rooms ... completely gone", Inspector Lawrence said.
More than 50 firefighters battled the blaze.
NSWFR trucks from Goulburn, Crookwell, St Andrew's, Moss Vale and Busby were tasked to the incident. Rural Fire Service crews also attended.
The sound of collapsing masonry could be heard from within the building, as roof tiles fell inward, leaving the timber frame skeleton exposed.
Street neighbour Phillip Phelps told Fairfax Media he was forever ringing the police about people in the building and the sounds of damage from within.
Christine McLaughlin, who lives across the road from the former boys' home, said she could often hear the sound of windows smashing in the property.
Former residents have described the fire as "incredibly sad, devastating but not unexpected".
"Like most people in Goulburn, all the 'old boys' have been expecting this fire," Phil Merrigan said.
"I have already received calls from some of the Old Boys and they are most upset. One of the boys mentioned to me how the Sisters at St John's instilled a high level of respect for other people's property and how important it was to do the right thing by people. They cannot understand how this could happen.
"The destructive state of the building and the fact that no one claimed to own the responsibility to repair or save it, have greatly contributed to this fire and they should all hang their heads in shame."
