Locals dug deep into their pockets on Friday night to donate €1.6 million to Puttinu Cares during a Good Friday fundraiser on TV show Xarabank.
That money will be combined with a €5 million donation Prime Minister Joseph Muscat pledged to Puttinu Cares on the government's behalf, with the money coming from the cash-for-passports Individual Investor Fund.
Puttinu Cares, which provides accommodation for the families of Maltese receiving medical treatment in the UK, is seeking to build 30 apartments in central London to make available to the families of patients.
Around 90 local patients travel to the UK with their families every month for medical care.
Xarabank host Peppi Azzopardi worked tirelessly to urge people to call in with their donations, and the response led to last year's €1.3 million donation figure being eclipsed, with €1,620,530 raised.
As the audience began celebrating reaching the €1.3 million mark, Mr Azzopardi took a phone call from Dr Muscat, who is currently in Australia to attend the Commonwealth Games opening.
Dr Muscat recalled how, when his father needed treatment in the UK many years ago, his family had been put up by nuns living there, saying he was well aware of how important the service they offered was.
The Prime Minister then pledged a €5 million donation on the government's behalf.
With more than €6.6 million raised, Puttinu Cares can now begin the search for land or apartments in central London.
In a statement, the NGO thanked people for their generosity and expressed its appreciation to the Office of the Prime Minister for its help.