Three kinds of needle coke (numbered as Coke-N, Coke-H and Coke-P) from different sources were studied with X-ray diffraction (XRD), Raman spectrum and curve-fitting analysis. The graphitization degree, crystal structure types and crystal size (La and Lc) of these three needle cokes were calculated with XRD. According to the curve-fitted analysis of XRD, the content of ordered crystallite structure (Ig) on the three needle coke samples was obtained. The graphitization degree of Coke-N and Coke-P were similar, which were obviously greater than that of Coke-H; the relationship of La between these needle cokes are: Coke-N＞Coke-P＞Coke-H. Raman spectrum coupled with curve-fitted method was used for quantitative analysis of samples. With Raman spectrum and math method, the cokes at zone of 1 000~2 000 cm-1 had been analyzed with curve-fitted method. This first-order spectrum had been curve-fitted to five peaks (G, D1, D2, D3, D4). The area of each fitted curve was used to calculate the distribution of carbon crystalline. The parameters of IG/IAll, ID1/IG, ID2/IG, ID3/IG and ID4/IG had shown that, the crystallite structure of Coke-N and Coke-P were more order than Coke-H. The ratio of ideal microcrystalline graphite carbon in Coke-N was 033, but the parameters of Coke-H and Coke-P were 0086 and 0311 respectively. What’s more, the ratio of amorphous carbon in Coke-H was obviously higher than other that of two samples. The results were corresponding to that of XRD analysis. Therefore, XRD and Raman spectrum analysis was an important method to judge the essence of coal-based needle cokes with different macro quality on the microcosmic level.