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PVDF-based polymers have garnered significant attention in the field of high-power density electrostatic capacitors due to their exceptional dielectric strength. However, their practical applications are constrained by low charge-discharge efficiency (η) and energy storage density (U e), which stem from high ferroelectric relaxation and low breakdown strength (E b). Here, a hydrogenated glassy polymer poly(styrene-methyl methacrylate-methylallyl alcohol) (PSMA) is designed and synthesized to be homogeneously distributed in PVDF through voltage-assisted 3D printing-hot pressing, resulting in a flexible composite film. The findings demonstrate that PSMA, rich in hydrogen bonds and high modulus strength, effectively mitigates the ferroelectric phase transition of PVDF to enhance η. Additionally, the voltage-assisted 3D printing process induces an entropy gain mechanism, facilitating the uniform distribution of the two phases and enhancing the interfacial properties for enhancing E b. Remarkably, the study achieves prominent growth in energy storage performance, with U e and η reaching 18.1 J/cm3 and 80 % at 525 MV/m, respectively. These remarkable results highlight the potential of 3D printing technology in enhancing the energy storage performance of PVDF-based dielectrics. Hydrogenation reduction and voltage-assisted 3D printing induces phase transitions in all-organic polymer composite films as well as enhance interfaces to enhance charge-discharge efficiency (η) and energy storage density (U e). [Display omitted] • Preparation of high modulus strength, polar group-rich linear polymer PSMA via polymerization and hydrogenation reduction. • Hydrogenation and voltage-assisted 3D printing induces phase transitions in composite films as well as enhance η and E b. • Unraveling the role of force-electric field on the phase transition of PVDF composites in voltage-assisted 3D printing. • The optimized PVDF/PSMA composites have significantly enhanced energy storage performance (525 MV/m, 18.1 J/cm3 and 80 %). [ABSTRACT FROM AUTHOR]