Although silicon (Si) has a high theoretical capacity, the large volume expansion during lithiation has greatly hindered its application in high-energy-density lithium-ion batteries (LIBs). Among the strategies for improving the performance of Si anode, the role of binders should not be underestimated. Here, a novel strategy for designing a cross-linkable binder for Si anode has been proposed. The binder with hydroxyl and nitrile groups can be in situ covalently cross-linked through the amide group in the batteries. The cross-linked binder (