Supercritical fluid (SCF) technology has become an important tool of materials processing in the last two decades. Supercritical CO2 and H2O are extensively being used in the preparation of a great variety of nanomaterials. The greatest requirement in the application of nanomaterials is its size and morphology control, which determine the application potential of the nanoparticles, as their properties vary significantly with size. The aim of this chapter is to provide a critical review of the recent advances in the use of supercritical fluids for the preparation and control of specific physical forms of pharmaceutical substances with particular attention to those used for the preparation of drug delivery systems.