Absolute Return for Kids or Ark, was set up by Arpad "Arki" Busson, the French multi-millionaire financier and father of supermodel Elle Macpherson's two children, is famous for lavish fundraising auctions, one of which made Pounds 11.1m in five hours.
Now some of that money is to be used to sponsor academies in Westminster, Hammersmith, Lambeth and Southwark.
Last year Ark withdrew from a scheme to replace Islington Green secondary and Moreland primary, in Islington, with the academy for three to 18-year-olds, saying that running an all-age school on a split site was too complex.
The charity still favours the all-age concept and two of the planned academies will fit the model.
But it regards breaking down large schools into smaller manageable units of no more than 400 pupils as a higher priority.
At Elephant and Castle, Southwark, the 1,622-pupil academy planned to replace Geoffrey Chaucer technology college and Joseph Lancaster primary in 2008 will effectively be six schools in one.
It will comprise a nursery and infant school, a junior school, two parallel 11-14 schools and two 14-19 schools each with their own heads and deputies answering to an overarching principal and specialising in music and the performing arts.
Ark has also been influenced by American charter schools and employed Jay Altman, a teacher who pioneered them in New Orleans in the early 1990s, as its education director.
He will oversee a new 3-18 academy due to open in Westminster in September.
With just two forms of entry it will operate on a site currently used by North Westminster community school.
In Hammersmith, Ark is to sponsor an 11-18 academy, run in partnership with the diocese of London, due to replace the failing Burlington Danes CE 11-16 school in September. The charity hopes to open an 11-18 academy in Brixton in 2008 following lobbying by the Secondary Schools Campaign In Lambeth , a parents' group calling for new local secondaries.
Plans for a further two Ark academies are to be submitted for government approval.
Eventually it aims to have seven in the capital with the possibility of more outside.
The charity, which has previously concentrated on combating HIV in Africa and helping Romanian orphans, raised pound;10m at a glitzy dinner in London in 2004, where guests bid vast sums for lots that included pound;160,000 for a tennis match with Tony Blair.
Last year's event at Battersea power station topped that making pound;11.1m, including pound;220,000 for a place on one of Virgin's first space flights and pound;120,000 for a training session with Chelsea stars Frank Lampard and John Terry.