Some FeS2 samples among metamorphic belt between coal and intrusion from Wolonghu mine in the north of Anhui Province were retrieved to characterize the signature of Raman Spectral. The results show that, all Raman data of different samples can be divided into 3 types as Ⅰ, Ⅱ and Ⅲ according to distinct differences of in Raman mode (M), Raman shift (Δν) and scattering intensity (Ⅰ). There are five strong scattering modes including high value Eg (1.16~1.59×103), high value Ag (2.33~2.53×103) and low value Tg (0.20~0.27×103) in typeⅠand only former three modes in type Ⅱ although the value of Eg, Ag and Tg are similar between them. While there are only two modes of high value Eg about 327.6~328.8 cm-1 and low value Ag 389.0~390.1 cm-1. Our analyses indicate that type Ⅰ samples must be mixed crystal of pyrite and natural coke for the former three peaks are same to deformation and stretching vibration of Fe-［S2］2- and stretching vibration of S—S in pyrite, while the latter two are similar to the vibration of Tiny graphite crystals and stretching vibration of C—C among graphite crystal from Raman data. And typeⅡsample may be pyrite for typical pyrite Scattering peak and Type Ⅲ sample possibility are low-temperature crystalloblastic of pyrite for Marcasite spectrum features in Raman. Further analysis also showed that the formation pressure of typeⅠ and Ⅱ are the same while type Ⅲ samples formed in low pressure for Raman scattered intensity of typeⅠand Ⅱ are similar, and type Ⅲ samples is obviously lower than the former two. And the formation temperature of typeⅠ, typeⅡ and type Ⅲ significantly decreased in turn for Ag peak of them are turn to high frequency about 4.4~6.7, 4.5~8.4cm-1 respectively compared with the former. Thus, The authors’ studies suggest that pyrite samples from Metamorphic coal and metamorphic zone in Wolonghu coal mine are products in high temperature, but samples from Magmatic rocks are Marcasite formed at low temperature.