For the fabrication of the Si negative electrode in Li-ion batteries (LIBs) containing the cross-linking polymer binder, in this work, the urethane acrylate (UA) oligomer was synthesized via a simple synthetic process. The cross-linked poly(urethane acrylate) (CPUA)/carbone black (CB)/Si composite (CPUA/CB/Si composite) was fabricated through reactions between their reactive vinyl segments in the UA oligomer. Interestingly, the CPUA/CB/Si composite showed better cycle performance than the poly(vinylidene fluoride) (PVdF)/CB/Si composite (PVdF/CB/Si composite) and the polyurethane (PU)/CB/Si composite (PU/CB/Si composite). The CPUA/CB/Si composite had the best lithiation of about 2586 mAh g-1. The UA oligomer showed a good compatibility with the electrode materials and current collector after and before a curing process.