Hybrid materials containing inorganic nanoparticles and p-conjugated polymers have unique properties and the internal organization of such materials on the nanometer length scale is often crucial in determining the desired properties. An attractive approach to control this organization involves self-assembly. For this aim several oligo(p-phenylene vinylene) (OPV) chromophores bearing a disulfide functionality were synthesized, functionalized onto gold nanoparticles and fully characterized. Optical spectroscopy studies including ultra fast pump-probe spectroscopy revealed that energy transfer occurred from the molecules to the metal core. Subsequently, OPV-capped gold nanoparticles were reversibly self-assembled by a solvent-directed method into micrometer-sized fractal-like spherical aggregates. This was proven by dynamic light scattering and optical studies in solution and TEM and AFM experiments in the solid state. Furthermore, a template-directed self-assembly approach was developed in which OPV-gold nanoparticles were homogeneously incorporated into a p-conjugated OPV gel fiber which served as a template.