A binder/additive free composite electrode of lithium iron phosphate/reduced graphene oxide with ultrahigh lithium iron phosphate mass ratio (91.5 wt% of lithium iron phosphate) is demonstrated using electrophoresis. The quasi-spherical lithium iron phosphate particles are uniformly connected to and/or wrapped by three-dimensional networks of reduced graphene oxide nanosheets, with intimate contact formed between the two. Enhanced capacity is achieved in the electrophoretic composite cathode, when compared to either the conventional one or composite cathode formed by mechanically mixing lithium iron phosphate and reduced graphene oxide. The present methodology is simple and does not disturb the active material growth process. It can be generally applied to a variety of active material systems for both cathode and anode applications in lithium ion batteries.