Dielectric capacitors are essential components of modern advanced electronic devices and power systems based on their ultra-fast charging and discharging speeds and supreme power densities. Nevertheless, how to comprehensively boost their energy storage density and storage efficiency is still an insurmountable challenge. Here, we report a simple micro-chemical polarizability modulation strategy that enables SrTiO3-based dielectric materials to achieve excellent energy storage properties. The energy density and energy efficiency are increased to as high as 76 J∙cm−3 and 72 % from 0.4 J∙cm−3 and 46.7 % of pure STO, respectively, which is the largest value in micro-substitution (less than 3 %). Our results show that the introduction of trace amounts of elements with high ionic polarizabilities (Mn, V) facilitates the increase of chemical disorder and the formation of stable and highly dynamic polar nanoregions (PNRs), which reduces the hysteresis of the polarization switching and improves the polarization at the breakdown field strength, synergistically fostering the energy storage performance. The results of X-ray photoelectron spectroscopy and scanning electron microscopy reveal that the micro-substitution of Mn and V promote the reduction of oxygen vacancies and grain size, improving the breakdown resistance and stability of the capacitor. This present approach is expected to be widely used in the development of high-performance dielectrics.