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Abstract A new polymer electrolyte based on holographic photopolymer is designed and fabricated. Ethylene carbonate (EC) and propylene carbonate (PC) are introduced as the photoinert substances. Upon laser‐interference‐pattern illumination, photopolymerization occurs within the constructive regions which subsequently results in a phase separation between the photogenerated polymer and unreacted EC–PC, affording holographic photopolymer electrolytes (HPEs) with a pitch of ≈740 nm. Interestingly, both diffraction efficiency and ionic conductivity increase with an augmentation of the EC–PC content. With 50 wt% of EC–PC, the diffraction efficiency and ionic conductivity are ≈60% and 2.13 × 10−4 S cm−1 at 30 °C, respectively, which are 60 times and 5 orders of magnitude larger than the electrolyte without EC–PC. Notably, the HPEs afford better anisotropy and more stable electrochemical properties when incorporating N,N‐dimethylacrylamide. The HPEs exhibit good toughness under bending, excellent optical transparency under ambient conditions, and astonishing capabilities of reconstructing colored images. The HPEs here open a door to design flexible and transparent electronics with good mechanical, electrical, and optical functions.