Hierarchical nanostructures containing three-dimensional (3D) spheres are promising materials due to their unique physicochemical characteristics. In this study, a 3D hierarchical walnut kernel shape conducting polymer binder (CPB) is facilely fabricated via emulsion polymerization method. CPB exert beneficial properties as a good adhesive for LiFePO4 cathodes, and an efficient conducting material for Li+ inside the cathode, providing a facile pathway for ion movement. Unlike one-dimensional (1D) binders, the unique 3D hierarchical structure exhibits multi-dimensional bonding interactions with active materials and therefore offers robust contacts between both components. When the active material loses its original contact with the binder during potential cycling, CPB can successfully recover its 3D hierarchical network, thus creating a self-healing effect. CPB-based LiFePO4 electrode shows remarkedly improved electrochemical performances compared to other well-known binders, such as poly(vinylidene fluoride).