One- and two-dimensional carbon nanomaterials were tested as adsorbents for the elimination of two anionic dyes, reactive red 2 and methyl orange, and the cationic dye methylene blue from aqueous solutions under the same conditions. Carbon nanomaterials performed well in the removal of dyes. Surface oxygenated groups in the nanomaterials improved the cationic dyes’ adsorption, but not the adsorption of the anionic dye. The interactions between nanomaterials and dyes were verified by infrared and Raman spectroscopy. The pseudo-second order kinetic model was better fitted to the kinetic experimental data than the Elovich and pseudo-first order models. The equilibrium adsorption data were best fitted by the Langmuir model. The dimensions and morphology of the carbon nanomaterials play an important role in the adsorption of the three dyes. The main mechanism of adsorption of anionic dyes is by the interactions of the aromatic rings of the dye structures and π delocalized electrons on carbon nanostructures; the adsorption of cationic dye is mainly due to electrostatic interactions.