Polymer Electrolytes In article number 2203413, Chang Yun Son, Moon Jeong Park, and co-workers establish a platform for innovative electrolyte technologies to achieve superionic conduction from solid-state polymer electrolytes. Through the rational design of bifunctional polymers capable of unique intra-monomer hydrogen bonding, interconnected rod-like ion channels are formed in the glassy polymer matrix, which enables a high ionic conductivity of 10−3 S cm−1 and high storage modulus of ca. 100 MPa at 25 °C.