The decoration included furniture bought or made specially for the villa, by Mallet-Stevens himself with his armchair « Transat » created for the swimming pool, by Djo-Bourgeois, Francis Jourdain, Pierre Legrain, Pierre Chareau, Jean Prouvé, Eileen Gray, Charlotte Perriand, Dominique (Marie André Domin), Sybold van Ravesteyn and Theo van Doesburg from De Stijl, the Wassily Chair of Marcel Breuer, or from the brands Smith & Co and Ronéo, as well as textiles by Raoul Dufy and Sonia Delaunay, luminaires by Jean Perzel, ironworks by Claudius Linossier, stained glass by Louis Barillet and pieces of art : sculptures by Jean and Joël Martel, Henri Laurens, Constantin Brâncuși, Alberto Giacometti, Jacques Lipchitz, paintings by Mondrian or Braque, etc.

Throughout the 1920s and 1930s, the couple were important patrons of modern art, particularly surrealism; they supported film projects by Man Ray, Salvador Dalí, and Luis Buñuel; and commissioned paintings, photographs and sculptures by Balthus, Giacometti, Constantin Brâncuși, Miró, and Dora Maar.

Villa Noailles features prominently in Man Ray's film Les Mystères du Château de Dé.

In his book Picasso and Dora: a memoir he writes: "...an undistinguished cubist extravaganza of reinforced concrete set atop a high hill, within the ancient walls of a Saracen fortress.

He recalls the room, where Marie-Laure tried to seduce him: "...a large salon at Saint-Bernard which had no windows but was lighted from above by a bizarre cubist skylight which occupied almost all the ceiling, adding to the sense of existing outside time in a stranded ocean liner."