A compensation method was proposed for correcting wheel setting error and residual form error in nanogrinding of axisymmetric surfaces. In this method, profile data from on-machine measurement were used to obtain the setting error of grinding wheel, as well as the normal residual form error. Compensation model of single-point inclined-axis grinding was built up for generating new compensation path. Grinding test of aspheric tungsten carbide mould was conducted to evaluate performances of the compensation method. A profile error of 182 nm (peak to valley) and average surface roughness of 1.71 nm were achieved. These results indicated that the form error compensation method may significantly improve form accuracy of ground surface.