Measurement of the interaction force between two materials provides important information on various properties, such as adsorption, binding, or compatibility for coatings, adhesion, and composites. The interaction forces of zwitterionic and ionic monomers with graphite platelets (G) and reduced graphene oxide (rGO) surfaces were systematically investigated by atomic force microscopy (AFM) in air and water. The monomers examined were 2-(methacryloyloxy)ethyl 2-(trimethylammonio)ethyl phosphate (MPC), [2-(methacryloyloxy) ethyl] dimethyl-(3-sulfop ropy1)ammonium hydroxide (SBE), [2-(acryloyloxy)ethyl]trimethylammonium chloride (ATC), and 2-methyl-2-propene-1-sulfonic acid sodium (MSS). The AFM studies revealed that MSS and SBE monomers with sulfonate units have stronger interaction forces with G surface in air and that MPC and ATC monomers with quaternary ammonium units have higher interaction forces in water. In the case of rGO surface, the monomers with quaternary ammonium units showed stronger interactions regardless of the medium. These interactions could be rationalized by the interaction mechanism between the monomers with graphene surfaces, such as cation-pi for MPC and ATC and anion-pi for MSS and SBE. Overall, cation-pi interactions were effective in water, whereas anion ir interactions are effective in air with G surface. The adhesion values of MPC, SBE, ATC, and MSS on rGO were lower than the values measured on G surface. Among the monomers, MPC showed the highest dispersibility for aqueous graphene dispersions. Further, the adsorption of MPC on G and rGO surfaces was verified by high-resolution transmission electron microscopy and X-ray diffraction patterns.