Objective To investigate the correlation between anterior corneal surface shape (including corneal curvature, corneal height, and asphericity) and corneal higher-order aberrations. Methods In this cross-sectional study, 57 eyes of 57 myopic subjects were included. The mean spherical refractive error was (-3.88±1.12)D (range-1.50--6.00 D) and cylinder was (-0.59±0.58)D (range 0--3.50 D). Anterior corneal surface shape was measured with a Pentacam (Oculus, Wetzlar, Germany) and index of surface variance (ISV), index of height asymmetry (IHA), aspheric index (Q-value) and anterior comeal aberrations were analyzed. A Pearson correlation analysis was used to assess the correlations between ISV, IHA, Q-value and anterior corneal higher-order aberrations. Results ISV had a significantly positive correlation with corneal vertical coma (Z3-1) and horizontal coma (Z3+1) (r=0.389, P=0.003; r=0.594, P<0.001). A negative correlation was found between ISV and corneal spherical aberrations (Z40) (r=-0.400, P=0.002). ISV was positively correlated with comeal 3rd-order aberrations (S3) (r=0.683, P<0.001) but showed a negative correlation with corneal 4*-order aberrations (S4) (r=-0.373, P=0.004). IHA was positively correlated with comeal Z3-1 and S3 (r=0.446, P<0.001; r=0.445, P<0.001). The Q-value showed a significant positive correlation with comeal Z40 and S4 (r=0.849, P<0.001; r=0.761, P<0.001). A negative correlation was found between the Q-value and 5th-order aberrations (r=-0.280, P=0.035). Conclusion Comeal 3rd-order aberrations increase with comeal surface curvature variance. Comeal vertical coma increases with the asymmetry of comeal upper and lower height. Comeal spherical aberrations increase as the anterior comeal surface shows more oblateness.