Binders play a key role in maintaining the integrity of high-capacity silicon anodes, which otherwise experience serious capacity decay during cycling caused by huge volume variation of the silicon. With an aim to developing a highly efficient polymeric binder to mitigate this capacity decay, we present a novel binder synthesized from polyacrylic acid (PAA) and polymerized β-cyclodextrin (β-CDp) for Si anodes for the lithium-ion batteries. This PAA-β-CDp binder has a 3D network structure, which provides strong adhesion between the active material and the current collector. PAA-β-CDp binder makes silicon anode achieve a specific capacity of 2326.4 mAhg at the current density of 0.2 A g with a capacity retention of 64.6% after 100 cycles. The experimental results show that the PAA-β-CDp binder can effectively mitigate the huge volume change and improve the capacity and cycling performance of Si anodes.