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Controlling architecture of electrode composites is of particular importance to optimize both electronic and ionic conduction within the entire electrode and improve the dispersion of active particles, thus achieving the best energy delivery from a battery. Electrodes based on conventional binder systems that consist of carbon additives and nonconductive binder polymers suffer from aggregation of particles and poor physical connections, leading to decreased effective electronic and ionic conductivities. Here we developed a three-dimensional (3D) nanostructured hybrid inorganic-gel framework electrode by in situ polymerization of conductive polymer gel onto commercial lithium iron phosphate particles. This framework electrode exhibits greatly improved rate and cyclic performance because the highly conductive and hierarchically porous network of the hybrid gel framework promotes both electronic and ionic transport. In addition, both inorganic and organic components are uniformly distributed within the electrode because the polymer coating prevents active particles from aggregation, enabling full access to each particle. The robust framework further provides mechanical strength to support active electrode materials and improves the long-term electrochemical stability. The multifunctional conductive gel framework can be generalized for other high-capacity inorganic electrode materials to enable high-performance lithium ion batteries. [ABSTRACT FROM AUTHOR]