Here, we show that the capacity retention rate and Coulombic efficiency of silicon/graphite composite anodes are improved significantly when the electrode particles are strongly bonded to the current collector with the aid of a polymeric adhesive interlayer. The improved adhesion between the electrode film and the current collector, which was confirmed by the scratch test, effectively suppresses the evolution of the interphase as well as the charge-transfer resistance of the electrode during cycling. Thus, it can be concluded that maintaining a good electrical contact between the active material and the current collector is crucial for developing high-performance Si anodes for lithium-ion batteries.