Based on Zernike polynomial fitting, we propose an algorithm believed to be new for interferometric measurements of rotationally asymmetric surface deviation of optics. This method tests and calculates each angular surface by choosing specified rotation angles with lowest error. The entire figure can be obtained by superimposing these sub-surfaces. Simulation and experiment studies for verifying the proposed algorithm are presented. The results show that the accuracy of the proposed method is higher than single-rotation algorithm and almost comparable to the rotation-averaging algorithm with fewer rotation measurements. The new algorithm can achieve a balance between the efficiency and accuracy.