The development of solid polymer electrolytes for lithium battery applications is a challenge of profound technological significance. We have established a collaboration with the aim of understanding and designing improved polymer electrolytes that combines theoretical modeling, polymer synthesis, and experimental characterization. By studying diverse polymer chemistries, we have discovered that ion-solvation-site connectivity is an important feature of polymer electrolytes that is necessary for high lithium-ion conductance. We are employing this insight into search for improved polymer electrolytes, with promising early-stage results.