Pyrophyllite is a raw material of significant interest due to its large number of applications. Most of these applications require a thermal transformation of pyrophyllite; this thermal transformation implies the release of structural OH groups and the formation of new phases. In this paper, we report on the dehydroxylation of pyrophyllite and the reversibility of the process. A value of 224 +/- 16 kJ/mol for the dehydroxylation of pyrophyllite was obtained. In addition, it was observed that the partially or totally dehydroxylated pyrophyllite suffered a partial reversible rehydroxylation when cooled to room temperature. This rehydroxylation was substantiated by thermogravimetric measurements, while infrared spectroscopic studies showed that, during the rehydroxylation, the intensity of the OH band at 3675 cm-1 increased as two new bands at 3690 and 3702 cm-1 appeared. This rehydroxylation process was heavily influenced by the particle size of the pyrophyllite. Thus, smaller particles (< 1 mu m) showed a larger rehydroxylation percentage (about 12%), while the larger ones (20-40 mu m) showed a smaller percentage (about 1.6%). The extent of rehydroxylation also depended on the dehydroxylation temperature and reached a maximum value at 750 degrees C.