Graphitic nanomaterials such as graphene, carbon nanotubes (CNT), and C60 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 106, 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.