Cohesive carbon assemblies are prepared by obtaining a carbon starting material in the form of powder, particles, flakes, or loose agglomerates, dispersing the carbon in a selected organic solvent by mechanical mixing and/or sonication, and substantially removing the organic solvent, typically by evaporation, whereby the cohesive assembly of carbon is formed. The method is suitable for preparing free-standing, monolithic assemblies of carbon nanotubes in the form of films, wafers, or discs, having high carbon packing density and low electrical resistivity. The method is suitable for preparing adherent cohesive carbon assemblies on substrates comprising various materials. The assemblies have various potential applications, such as electrodes or current collectors in electrochemical capacitors, fuel cells, and batteries, or as electromagnetic interference shielding materials.