Wool, cotton and ramie thermal properties are qualitatively studied by temperature-dependent Fourier transform infrared (TD-FTIR) spectroscopy, and quantitatively investigated by thermogravimetry coupled with a differential thermal analyzer (TG-DSC). TD-FTIR results indicate that although cotton, ramie and wool exhibit significant water loss, they have no detected degradation within the temperature range from 25℃ to 210℃. These data are confirmed by TG-DSC analysis. Dynamic mechanical thermal analysis provides comparative study of cotton, ramie and wool bundles’ dynamic mechanical thermal properties. The four-fiber-bundle has a much lower storage modulus due to its larger fiber contact surface and twisting deformation; heating reduces the storage modulus significantly for cotton and ramie instead of wool fiber bundles in the temperature range from 25℃ to 100℃. Key E′-T and tan δ-T curve information reveals that ramie fiber bundles have the strongest temperature sensitivity, while wool fiber bundles express the weakest temperature sensitivity.