The aim of this work was the self-assembly of innovative composite particles by means of electrostatic layer-by-layer deposition. To prepare the composite particles, spherical nanoparticles were adsorbed on the surface of lamellar particles. As lamellar particle with a high surface potential and a high aspect ratio, positively charged layered double hydroxides was chosen. As spherical particles, negatively charged particles of silica and a synthesized electrosterically stabilized acrylate dispersion with 1,1-diphenylethylene were selected. The deposition of the particles by the LbL-technique was characterized on charged surfaces. Based on gained knowledge of deposition behaviour, they were organized into novel composite particles. SEM images showed a complete coverage of the LDH surface by silica particles. A stabilization of delaminated LDHs in aqueous media could be achieved by using silica particles. By adsorption of DPE dispersion on the LDHs a uniform deposition of the particles was observed with a regular constant distance between the individual particles. In the last part of this work, stacked colloids were produced in two different routes. The first was the electrostatic deposition of the preorganized particles and re-addition of LDH. In the second variation, stacks were formed directly by addition of spherical particles to LDH. The colloids were incorporated into a polymer matrix. Subsequent SEM analysis of the FIB cross section confirmed the successful stacking of the colloids.