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Novel sunflower-like organic–inorganic composites consisting of spherical silica and smaller conductive polypyrrole particles were successfully prepared through an in situ self-assembly polymerization process by choosing chitosan as a modifying agent of silica surface. Transmission electron microscopy (TEM) and scanning electron microscopy (SEM) showed that on the surface of individual silica particle polypyrrole nanoparticles were anchored perfectly. The sunflower-like silica–polypyrrole composites exhibited conductivity of 8Scm −1 and colloid stability because of the special surface morphology. Adsorbed chitosan chain may play a dual-role of both providing the active sites for formation of the polypyrrole particles on silica and acting as a stabilizer of the silica–polypyrrole particles. Hydrogen-bonding interaction between the acetylamino group of chitosan and hydrogen atom on nitrogen of polypyrrole is a determining parameter in the former case.