Synergetic Lithium and Hydrogen Bonds Endow Liquid‐Free Photonic Ionic Elastomer with Mechanical Robustness and Electrical/Optical Dual‐Output

. Meanwhile, the synchronous electrical and optical output under mechanical strains can be achieved in the PIEs with the presence of dissociated ions contributed by lithium bond and non-close-packed SiNPs stabilized by the hydrogen bond. Moreover, due to their liquid-free nature, the PIEs exhibit extraordinary stability and durability, which can withstand extreme conditions including both high and low temperatures as well as high humidity. This work provides a promising molecular engineering route to construct high-performance photonic ionic conductors toward advanced ionotronic applications.