A sequential particle assembling process was developed to fabricate composite particles with multiple components. Cobalt sintering aids and carbon nanotube (CNT) conductive additives were sequentially and electrostatically absorbed on Li1.3Al0.3Ti1.7(PO4)3 (LATP) electrolyte particles under various dispersion conditions. The effect of the particle assembling conditions on the composite body's sintering ability and conductive properties was investigated. By optimizing the microstructure of the composite particle and its particle charging conditions, it became possible to obtain a sintered composite electrode with a finely connected path of each LATP and CNT phase.