BaTiO₃-based lead-free ferroelectric films with a large recoverable energy density (W_rec) and a high energy efficiency (η) are crucial components for next-generation dielectric capacitors, which are used in energy conditioning and storage applications in integrated circuits. In this study, grain-engineered (Ba_0.95,Sr_0.05)(Zr_0.2,Ti_0.8)O₃ (BSZT) ferroelectric thick films (~500 nm) were prepared on Si substrates. These films were deposited at 350 °C, 100 °C lower than the temperature at which the LaNiO₃ buffer layer was deposited on Pt/Ti. This method reduced the (001) grain population due to a weakened interface growth mode, while promoting volume growth modes that produced (110) and (111) grains with a high polarizability. As a result, these films exhibited a maximum polarization of ~88.0 μC/cm², a large W_rec of ~203.7 J/cm³, and a high energy efficiency η of 81.2% (@ 6.4 MV/cm). The small-field dielectric constant nearly tripled as compared with that of the same BSZT/LaNiO₃ heterostructure deposited at the same temperature (350 °C or 450 °C). The enhanced linear dielectric response, delayed ferroelectric polarization saturation, and increased dielectric strength due to the nano-grain size, collectively contributed to the improved energy storage performance. This work provides a novel approach for fabricating high-performance dielectric capacitors for energy storage applications.