We observed that thermally treated carbon nanowalls serve efficiently as templates governing the formation of quasiperiodic patterns for nanoparticles deposited. Here we report self-assembled quasi-regular structures of diverse nanoparticles on a freestanding multilayer graphene-like material, i.e. carbon nanowalls. Metallic (Ag, Al, Co, Mo, Ni, and Ta) and semiconductor (Si) nanoparticles form coaxial polygonal closed loop structures or parallel equidistant rows, which evolve upon further deposition into bead-like structures and, finally, into nanowires. Weakly bonded nanoparticles decorate atomic steps, wrinkles and other extended defects on the carbon nanowalls as a result of anisotropic diffusion of atoms or clusters along the hexagonal sp2-carbon network followed by their aggregation and agglomeration. The decorated carbon nanowalls are found to be promising materials for surface enhanced Raman scattering (SERS) analysis.