Raman spectroscopy has, for long, been utilized to investigate material systems on the micro and mesoscales. Recently, the technique has proven its ability in exploring systems on the nanoscale. In this paper, we review our recent work on the Raman investigation of molecular adsorption from liquid mixtures on surfaces of single-walled carbon nanotubes and fullerene nanospheres, emphasizing the following major research findings: the development of a Raman-based technique capable of sensing local chemical interactions on the surface of carbon nanotubes and spheres; the molecular simulation results supporting the Raman investigation; the possibility of creating mesostructures based upon mixtures of carbon nanotubes and nanospheres that are crucial for selective adsorption. The current findings represent a major new thrust for the development of new nanostructured materials with superior adsorption capabilities and unique applications.