Based on the field investigation of painted sculptures in Yunlin Temple of Yanggao County, the chemical compositions of pigments were analyzed using XRD, XRF, SEM-EDS, Raman spectrometry and other methods. It was found that painted sculptures in Yunlin Temple were made following a traditional process, but also had something special, such as paper mounting, use of mixed pigments and gold scratching, etc. Red pigments were red lead, cinnabar and iron red; green, Paris green and basic copper chloride; blue, azurite and ultramarine; and the black one, carbon black. This research comprehensively reveals the manufacturing techniques and materials for painted sculptures in the Great Buddha’s Hall of Yunlin Temple, enriches the understanding of the manufacturing techniques and materials for ancient painted sculptures, and lays a foundation for the implementation of conservation and restoration.