Objective: To determine the pyrolysis characteristics of calcined and processed calamine, qualitatively and quantitatively compare the contents of related elements, morphology and functional groups of the pyrolysis products dried at different heating temperatures and explore the critical temperature and the optimal drying temperature for the process of calamine with Huanglian Decoction(HLD, 黄连汤) and San Huang Decoction(SHD, 三黄汤). Methods: Pyrolysis products were prepared by programmable and constantly heating the calcined and processed calamine to or at different heating temperatures. Thermogravimetry(TG) was used to test their pyrolysis characteristics. Fourier transform infrared spectroscopy and scanning electron microscopeenergy dispersive spectrometer were used to determine their morphology, functional groups and element contents. Page model was used to investigate the constant drying kinetics of processed calamine. Results: The adding of HLD or SHD to calcined calamine(CC) can slow its weight loss in drying pyrolysis process. The temperature ranges where HLD and SHD can affect its weight loss were 65–150 ℃ and 74–180 ℃, respectively. The drying temperature was optimized as 90 ℃. The drying kinetic for the processed calamine fits Page model shows good linearity. Conclusions: The critical temperature and the optimal drying temperature where HLD and SHD can affect the weight loss rate in the process of calamine were explored using the theories and methods of both biophysical chemistry and processing of Chinese materia medica. This work provides a good example for the study of the process of other Chinese medicines using modern analytical techniques.