Cross-linked polymers generated from low molecular weight oligomers were investigated for the first time as electrode binders in lithium-ion batteries. With urethane acrylate-based binder precursors, electrode laminates of LiNi1/3Mn1/3Co1/3O2 (NMC) with good physical properties were prepared via a thermally initiated free-radical polymerization process. The cured NMC electrode was evaluated in both NMC/Li and NMC/MCMB cells and showed excellent cycling performance and C-rate capability.