LAUSR

The development of advanced solid‐state energy‐storage devices is contingent upon finding new ways to produce and manufacture scalable, high‐modulus solid‐state electrolytes that can simultaneously provide high ionic conductivity and robust mechanical integrity. In this work, an efficient one‐step process to manufacture solid polymer electrolytes composed of nanoscale ion‐conducting channels embedded in a rigid crosslinked polymer matrix via Digital Light Processing 3D printing is reported. A visible‐light‐mediated polymerization‐induced microphase‐separation approach is utilized, which produces materials with two chemically independent nanoscale domains with highly tunable nanoarchitectures. By producing materials containing a poly(ethylene oxide) domain swelled with an ionic liquid, robust solid polymer electrolytes with outstanding room‐temperature (22 °C) shear modulus (G’ > 108 Pa) and ionic conductivities up to σ = 3 × 10−4 S cm−1 are achieved. The nanostructured 3D‐printed electrolytes are fabricated into a custom geometry and employed in a symmetric carbon supercapacitor, demonstrating the scalability of the fabrication and the functionality of the electrolyte. Critically, these high‐performance materials are manufactured on demand using inexpensive and commercially available 3D printers, which allows the facile modular design of solid polymer electrolytes with custom geometries.