The formation of macroscale carbon structures characterised by an sp-sp ²-hybridization is realised by self-assembly in colloidal solutions under an effect of laser irradiation and electromagnetic fields. The sponge-like morphology, sculptured with gold nanoparticles (NPs) was revealed by Scanning Electron Microscopy (SEM) imaging. Full structural and defect characterization of the self-assembled sponges was provided using the micro-Raman spectroscopic technique. The synthesized clusters manifest themselves in the presence of a strong spectral band in the visible range of the photoluminescence spectra that is quite unusual for ordered sp ²-carbon systems.