Savills, the property agents, expect a price of between pounds 10m and pounds 15m for Mentmore Towers in Buckinghamshire and its 81-acre grounds.
The Maharishi Foundation, an educational charity which works under the guidance of Maharishi Mahesh Yogi, has had its headquarters at the 19th century house since 1978.
The Natural Law Party, whose yogic flying candidates have highlighted the teachings of the Maharishi in the last two general elections, also rent rooms there.
Dr Geoffrey Clements, of the foundation's trustees, said Mentmore had been a "superb home" and they would be sad to leave. But he added: "The success we are experiencing with our activities means we are looking for a new home."
The building was designed by Sir Joseph Paxton, the man who designed Crystal Palace, and built for Baron Myer Amschel de Rothschild in 1855.
It passed to Hannah Rothschild who married the 5th Earl of Rosebery, who was prime minister in 1894-95. But when the 6th Lord Rosebery died in 1974, the 7th Earl, Neil Archibald Primrose, faced considerable duties.
He offered the house and its treasure trove of art and antiques to the Government in lieu of duties for a reported sum of pounds 3m.
But the Government refused, provoking a storm of protest. Sotheby's arranged an auction of the contents in May 1977 which became known as "the sale of the century".
What was arguably the finest private collection of continental art and antiquities in the country was sold for pounds 6m in nine days. Part of the estate was also sold to become the Mentmore golf and country club.
The house includes a grand hall, five state and major reception rooms, seven bedroom suites and around 50 more bedrooms. Many rooms have ornate gilt work and wooden panelling - the most splendid of which is the dining room, lined with 18th century gilded boiseries, originally designed for the French royal house, and panels of Genoese velvet bought from the Duke of Buckingham at Stowe. The style is Italian palazzo in the public areas and French Versailles in the reception rooms.
There is a series of fine marble fireplaces originally imported from the Continent, including an enormous marble chimney piece in the central hall. This was reputed to have been designed by Rubens for his home in Antwerp.
Ian Stewart, for Savills, said: "This is a magnificent stately house, probably the most important to be offered in 1997. It is rare for a property of this calibre to be offered on the market."
Part of the Maharishi Foundation's expansion will include taking in up to several hundred students for its newly-formed Maharishi College of Management and Technology which runs courses approved by London University.