Perpendicular magnetic anisotropy (PMA) plays a critical role in spintronics, giving rise to improvements in fundamental research and industrial production. Generally, PMA originates mainly from the spin-orbit interaction with perpendicular orbital moment. However, electron orbitals are difficult to tune once they emerge. Here, we propose a simple and effective method for preparing (001)-oriented ultrathin La0.67Sr0.33MnO3 (LSMO) films with PMA, which is induced by compressive strain and surface symmetry breaking. Moreover, PMA was effectively strengthened by means of annealing under applied magnetic field. X-ray linear dichroism spectra reveal that PMA should be attributed to the preferential occupancy of the 3z(2)-r(2) orbital in LSMO films. The results presented here show that PMA can be manipulated by orbital reconstruction in perovskite manganite films under compressive strain through a simple and effective strategy. These findings illustrate a new method for designing and controlling magnetic anisotropy and might advance fundamental applications of orbital physics and spintronics.