The present invention relates generally to electrolyte materials. According to an embodiment, the present invention provides for a solid polymer electrolyte material that has high ionic conductivity and is mechanically robust. An exemplary material can be characterized by a copolymer that includes at least one structural block, such as a vinyl polymer, and at least one ionically conductive block with a siloxane backbone. In various embodiments, the electrolyte can be a diblock copolymer or a triblock copolymer. Many uses are contemplated for the solid polymer electrolyte materials. For example, the novel electrolyte material can be used in Li-based batteries to enable higher energy density, better thermal and environmental stability, lower rates of self-discharge, enhanced safety, lower manufacturing costs, and novel form factors.