Thomas Sharkey Snr was being treated at Glasgow's Royal Infirmary More than 50 police officers are investigating what is now being treated as a triple murder inquiry.
Thomas Snr, 55, and his wife Angela, 46, were both taken to hospital in a critical condition.
Mr Sharkey died at Glasgow Royal Infirmary on Saturday morning.
He had initially been unaware of the deaths of his children, but his condition had improved enough for him to be informed on Tuesday.
The fire at the Sharkey family home in Helensburgh's Scott Court broke out at about 05:00 on Sunday.
Thomas Sharkey Jnr died in the blaze, while his sister Bridget died later in hospital.
Mr Sharkey was informed of the deaths of Bridget and Thomas Jnr Strathclyde Police have set up an incident room, dedicated phone line and email address for their murder inquiry.
The officer in charge of the investigation, Det Ch Insp Anne McKerchar, said officers had been encouraged by the response from the public, who were "clearly appalled at this cowardly and despicable crime".
"We are continuing to conduct door-to-door inquiries and are following a number of lines of inquiry," she said.
"We have always said that the key to this investigation will be someone in the community who knows who did this and the people in Helensburgh have responded to our call in great numbers."
The inquiry number for people to call is 01389 822162. The dedicated email address is: operationendeavour@strathclyde.pnn.police.uk
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