Zhihua Temple is one of the most typical temples built in early Ming Dynasty. It has great value of study thanks to the well-preserved buildings after the Ming, Qing, and Republican periods, combining with the architectural styles in Song and Yuan Dynasty.Three big stone carvings in the temple have obvious black pollutants on their surfaces. It is necessary to carry out scientific analysis and research on the unknown black pollutants, for the purpose of protecting stone historical relics effectively. The portable X-ray fluorescence spectroscopy (pXRF), Raman spectroscopy, Fourier-transform infrared spectroscopy (FT-IR) and pyrolysis gas chromatography-mass spectrometry (Py-GCMS) were used to analyze the composition of the contaminants. The results indicated that the pollutants were mainly composed of dry plant oil, as well as amorphous carbon and a small amount of protein residues. As for the black attachments on the back of the BiXi (Stone Turtle) in front of the Tathagata Hall, polysaccharides, lipids, amorphous carbon, cellulose, protein residues and quartz could be figured out through results. A scientific basis for identifying the black pollutants on the stone carvings in Zhihua Temple accurately was obtained by this study, which had a great significance for making an effective protection plan of related stone historical relics.