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Polymeric dielectrics have attracted intensive attention worldwide because of their huge potential for advanced energy storage capacitors. Thus far, various effective strategies have been developed to improve the inherent low energy densities of polymer dielectrics. However, enhanced energy density is always accompanied by suppressed discharge efficiency, which is detrimental to practical applications and deserves considerable concern. Targeting at achieving simultaneous high energy density and high discharge efficiency, the unique design of asymmetric all‐polymer trilayer composite consisting of a transition layer sandwiched by a linear dielectric layer and a nonlinear dielectric layer is herein reported. It is demonstrated that the nonlinear dielectric layer offers high energy density, while the linear dielectric layer provides high discharge efficiency. Especially, the transition layer can effectively homogenize the …