In order to understand the painting materials and profile structures used in the creation of Chinese ancient folk architectural paintings, the architectural paintings of the Bell and Drum Tower at Fushan Temple in Shaanxi Province of China was investigated. In this study, optical microscopy, Fourier transform infrared spectroscopy (FTIR), micro-Raman spectroscopy, scanning electron microscopy-energy-dispersive X-ray spectroscopy (SEM-EDS), and chemical experimental methods were used. The profile structures, and the elemental and chemical compositions of the pigments and binders in the ground layer of the 12 samples were determined. Results showed that the painting profile structures in both towers comprised of pigment layer, underpainting layer and ground layer, where no starch was found in the chalk ground layer. The pigment layer mainly comprised of iron oxide red, chalk, lapis lazuli, carbon black, green earth, and a dark green pigment that is formed by a combination of carbon black and green earth. To-date, the use of green earth pigment in Chinese architectural paintings was not found in Chinese related academic literature; hence, this study marked the first identification of green earth being used in the architectural paintings. Tung oil, commonly used in Chinese architectural paintings as a binder for pigment, was also identified in the samples. Results from this study will serve as an important reference for better scientific investigation methods on ancient Chinese folk painting materials.