We investigated the use of polymerized vinylene carbonate (polyVC) as a binder for graphite anodes in lithium-ion cells. It functions not only of a traditional binder, but also plays an important role in surface stabilization of graphite in propylene carbonate (PC)-based electrolytes. In an electrolyte with PC content as high as 30 wt%, the polyVC binder enhanced battery performance, with a reversible capacity of ∼170 mAh g−1 at a delithiation rate of 1 C, whereas a comparable graphite cell fabricated with a polyvinylidene fluoride (PVDF) binder failed to cycle.