It is important to identify pigments of painting and colored drawing in ancient architectures in order to restore and conserve them. The components of green pigments were detected with X-ray diffraction (XRD), X-ray fluorescence (XRF) and scanning electron microscopy-energy dispersive X-ray (SEM-EDX). Twenty-seven samples were collected from painting and colored drawing in northern Chinese ancient architectures in Beijing, Shanxi province and Gansu province. The experiment results showed that emerald green ［CuCH3COO］2? Cu(AsO2)2］, a complex of copper aceto-arsenite pigment, had been used as the colored component in fifteen samples, whereas organic materials synthesized in the rest. However, in all samples there were no malachite and atacamite, green pigments commonly used in ancient time a long time ago. These two pigments have been found in Qin Shihuang’s Terracotta Army and the wall paintings at Mogao Grettoes, Dunhuang, and some other famous wall paintings and color pottery figurines. However, emerald green was used many years later. It was reported that emerald green was synthesized by Germany in 1814 and had been widely used in China as watercolor on pith paper works and on scroll paintings since the 1850s. Because painting and colored drawing in ancient architectures stands outside, under sunlight and rain, it must be repaired and repainted in less than fifty years. Therefore, it is not surprising that emerald green was used in them. In recent years, artificial organic materials are increasingly used in painting and colored drawing in ancient architectures. From experiments it was also showed that in the same recolored painting and colored drawing, organic materials are usually in the later layers, but emerald green is in the earlier layers. This work supplies a lot of data for the purpose of selecting restoration materials and identifying painting and colored drawing in ancient architectures with a new method.