Advances in lithium battery technologies necessitate improved energy densities, long cycle lives, fast charging, safe operation, and environment-friendly components. In this study, we investigated lithium organic batteries comprising bioinspired polyvinyl catechol (P4VC) cathode materials and single-ion conducting polymer nanoparticle electrolytes. The controlled synthesis of P4VC resulted in a two-step redox reaction with voltage plateaus at ~3.1 and ~3.5 V as well as a high initial specific capacity of 352 mAh g -1 . The use of single-ion nanoparticle electrolytes enabled the synergistic achievement of high electrochemical stabilities up to 5.5 V, lithium transference number of 0.87, high ionic conductivities ranging from 0.2 × 10 -3 to 10 -3 S cm -1 , and stable storage moduli >10 MPa in 25-90 °C. Lithium cells can deliver 165 mAh g -1 at 39.7 mA g -1 for 100 cycles and stable specific capacity >100 mAh g -1 at high current density of 794 mA g -1 for 500 cycles. As the first successful demonstration of solid-state single-ion polymer electrolytes in environmentally benign and cost-effective lithium organic batteries, this work establishes a future research avenue for advancing lithium battery technologies.