Moso bamboo (Phyllostachys pubescens) and sinocalamus affinis (Phyllostachys heterocycla) were used in the research. Thermogravimetry (TG), a combination of TG and Fourier transform infrared spectrometer (TG-FTIR), X-ray diffraction (XRD), and differential thermal analysis (DTA) were used to investigate thermal decomposition of bamboo. The calorific value and smoke release process of both bamboos were also tested, respectively. The results from TG indicated that degradation process of sinocalamus affinis and moso bamboo was similar, but their degradation temperatures were different. The main decomposition occurred in the second step and about 68.70 and 64.63% masses degraded for sinocalamus affinis and moso bamboo, whose temperature of maximum mass loss was 319 and 339 A degrees C, respectively. DTA curve showed that the thermal decomposition of both bamboos was an absorbance heat process. TG-FTIR analysis showed that the main pyrolysis products of both bamboos were similar, including absorbed water (H2O), methane gas (CH4), carbon dioxide (CO2), acids and aldehydes, ammonia gas (NH3). The calorific value of moso bamboo (19,291 J g(-1) K-1) was higher than that of sinocalamus affinis (18,082 J g(-1) K-1). The initial time of smoke release process of moso bamboo was later, and its maximum smoke density was higher than that of sinocalamus affinis. The difference was probably attributed to different compositions and structure of sinocalamus affinis and moso bamboo. The results from this research are very helpful to better design manufacturing process of bio-energy, made from bamboo, by gasification and pyrolysis methods.