Graphitic nanomaterials such as graphene, carbon nanotubes (CNT), and C 60 fullerenes are promising materials for energy applications because of their extraordinary electrical and optical properties. However, graphitic materials are not readily dispersible in water. Strategies to fabricate all-carbon nanocomposites typically involve covalent linking or surface functionalization, which breaks the conjugated electronic networks or contaminates functional carbon surfaces. Here, we demonstrate a facile surfactant-free strategy to create such all-carbon composites. Fullerenes, unfunctionalized single walled carbon nanotubes, and graphene oxide sheets can be conveniently co-assembled in water, resulting in a stable colloidal dispersion amenable to thin film processing. The thin film composite can be made conductive by mild thermal heating. Photovoltaic devices fabricated using the all-carbon composite as the active layer demonstrated an on-off ratio of nearly 10 6, an open circuit voltage of 0.59V, and a power conversion efficiency of 0.21%. This photoconductive and photovoltaic response is unprecedented among all-carbon based materials. Therefore, this surfactant-free, aqueous based approach to making all-carbon composites is promising for applications in optoelectronic devices.