Enhancing the high electric field resistance and energy storage capacity of polymer dielectrics has been a long-standing challenge for the iterations of power equipment. Synergistic inhibition of carrier injection and transport is vital to energy storage performance improvement. Herein, promising polymer polyetherimide (PEI) was employed as a matrix and wider bandgap boron nitride nanosheets (BNNSs) were used as a reinforcing filler. Utilizing high-throughput stochastic breakdown simulations with the distribution characteristics of BNNSs as parameters, a series of topological gradient structures with the potential to enhance performance were obtained, thereby shortening the experimental cycle. Changing the BNNS distribution of symmetric/asymmetric and positive/inverse gradients, as well as the total and gradient contents of BNNSs, means that the position and condition of the surface barrier layer and central hinder layer change, which influences the energy storage performance of the polymer at room temperature and high temperature. Remarkably, the asymmetric gradient structure composite dielectrics exhibited excellent performances. Among them, the PEI-based composite dielectric with 2 vol% BNNS asymmetric inverse gradient distribution (gradient content of 1 vol%) achieved energy densities of 8.26 and 4.78 J cm-3 at room temperature and 150 °C, respectively. The asymmetric gradient structure design strategy holds great promise for optimizing the energy storage capacity of polymer dielectric capacitors.