The development of advanced pulse power technology proposes higher demand for dielectric energy storage materials. However, simultaneously obtaining high polarization and breakdown strength has become an obstacle to the development of dielectric materials. Herein, through the elaborate design of multivariant ions Me, BiMeO3 system thin film Bi(Ni0.5Zr0.5)O3 integrating high polarization, large breakdown strength and a localized heterostructure, generating an excellent energy storage density of 77.42 J cm−3 and efficiency of 70.29% at 5.60 MV cm−1. The enhancive breakdown strength of Bi(Ni0.5Zr0.5)O3 thin film is mainly attributed to the amorphous phase induced by low preparation temperature and the oxygen vacancy bound by the valence change of Ni2+ ion, which reduces leakage current density. This design approach is expected to be widespread for the development of BiMeO3 system thin film.