The HPLC fingerprints of Epimedium and Epimedii Wushanensis Folium were established, and quality evaluation was carried out by combining similarity analysis, chemometric methods, and grey relational analysis. Separation was performed on a Welch Xtimate^® C₁₈ column with gradient elution (0.1% of formic acid as mobile phase A, and acetonitrile as mobile phase B) at a flow rate of 1.0 mL/min, the column temperature of 30℃, and detection wavelength of 270 nm. The HPLC fingerprints of five types of Epimedium were established. Quality evaluation was conducted through similarity analysis, principal component analysis (PCA), partial least squares discriminant analysis (PLS-DA), and grey relational analysis. The results showed that high similarity in fingerprints of the same origin and good specificity of the established fingerprints. The results of PCA and PLS-DA showed that there were significant differences in chemical composition among different origins. Grey relational analysis identified Longnan City (Gansu Province) and Tonghua City (Jilin Province) as the the optimal production areas for E.brevicornu Maxim. and E. koreanum Nakai, respectively, among the tested samples. The integrated method combining fingerprinting, chemometrics and grey relational analysis provided an effective means for the quality evaluation of Epimedii Folium from different origins.