The magnitude of the dipole effect detected by the cutoff energy measurement was modulated for SrTiO3 (STO)/LaAlO3 (LAO)/SrRuO3 (SRO)/STO (001) subs. epitaxial stacks by ultrathin SrAlOx (SAO) insertion prior to LAO deposition. The difference in frictional forces on the LAO surfaces between the stacks with and without SAO insertion was clearly detected by lateral force microscopy (LFM), which indicated the change in dominating surface atomic layers. From the statistical analysis of LFM images, the SAO insertion was found to improve the lateral uniformity of the stacking sequence of charged monatomic layers in epitaxial LAO along the c-axis [(LaO)+ and (AlO2)−], taking account of the inevitable correlation between the surface-terminating atoms with the stacking sequence of the charged monatomic layers in epitaxial LAO. These results are consistently explainable with the proposed model that the interface dipole effect along the c-axis of the perovskite epitaxial stack is determined by the stacking sequence of charged monatomic layers of LAO.