Polyacrylates were applied as a binder of graphite electrode in a lithium-ion cell to modify the interface. Compared to a conventional binder, poly(vinylidene fluoride), the efficiency at the initial cycle was improved by poly(acrylic acid) and alkali polyacrylates in an ethylene carbonate (EC)-based electrolyte with highly reversible lithium intercalation. In a LiClO4 propylene carbonate (PC) solution, the poly(vinylidene fluoride) electrode showed a huge irreversible capacity as is generally known. However, the polyacrylate-modified graphite demonstrated highly reversible lithium intercalation in the PC electrolyte containing no film-forming additives as well as in the EC electrolyte due to the interfacial modification with polyacrylates.