A method for producing an organic-inorganic complex by intercalation of a positively charged organic compound between layers of a layered silicate, the method characterized by comprising the steps of heat-treating a hydrous layered silicate having a hydroxyl group in its crystalline structure at a temperature not higher than 1,200° C. and lower than the phase transition temperature of the silicate to dehydrate the silicate in Step (I);
- and allowing the dehydrated layered silicate to contact an aqueous solution containing a positively charged organic compound in Step (II).