Improving energy storage density and efficiency is the ultimate goal of dielectric materials used in ceramic capacitors. Among different dielectric materials, dielectrics in thin film state own superior energy performances due to less defects compared with ceramic. Herein, we report an optimized lead-free Zr-modified BiMg0.5Zr0.04Tix-0.04O3 composition with enhanced energy storage behavior via microstructural engineering. Rapid annealing can result in poorly crystallization in the film matrix confirmed by grazing incident X-ray diffraction GIXRD. The excess Ti source can effectively increase polarization and dielectric breakdown till to 97.0 μC/cm2 and 3403 kV/cm at x = 0.775, respectively. The optimized energy properties can be achieved at x = 0.775 with a high recoverable energy storage density Wreco of 87.8 J/cm3 and an efficiency η of 50%, indicative of excellent stability of storing electricity for the applications of pulse power electronics.