The electronic and ionic conductivity inside an electrode play a decisive role in cell performance of lithium-ion batteries (LIBs). However, traditional polymer binders connecting the conductive network for active material often tend to lose their original structure and function after the immersion of electrolyte. This will make the conductive network collapse, thus affecting charge/discharge capacity and cycle stability of LIBs. Here, Poly(amidoamine) (PAMAM) induced three-dimensional (3D) crosslinked polymer was designed and applied as a binder for LIB cathodes. Compared with conventional linear Polyvinylidene fluoride (PVDF) binder, the 3D binder exhibits better bonding ability and electrolyte affinity, which respectively bring superior electronic and ionic conductivity for LiFePO4 cathode so that the slighter polarization and better C-rate capability (140 mAh g-1 in 2 C discharge) are achieved. In addition, the cross-linked network constructed in the binder provides smooth and stable surface morphology for the electrode through stronger own strength and adhesion with substrate (average 7.69 N), which finally leads to improved cycling performance (98% retention after 250 cycles). Clearly, this 3D cross-linked polymer will bring new breakthrough for binder during the development of higher power LIBs.