In this study, single-chain atomic crystals (SCACs), Mo₃Se₃^-, which can be uniformly dispersed, with an atomically thin diameter of ∼0.6 nm were modified to disperse in an organic solvent. Various surfactants were chosen to provide steric hindrance to aqueous-dispersed Mo₃Se₃^- by modifying the surface of Mo₃Se₃^-. The organic dispersions of surface-modified Mo₃Se₃^- SCACs in nonpolar solvent (toluene, benzene, and chloroform) were stable with a uniform diameter of 2 nm, and they have enhanced stability from oxidation (>10 days). With the surfactants that have a polystyrene tail group (PS-NH₂), the surface-modified Mo₃Se₃^- SCAC showed high compatibility with a polystyrene polymer matrix. Using the surface-modified Mo₃Se₃^- SCAC, a homogeneous Mo₃Se₃^-/polystyrene/toluene organogel was prepared. More importantly, the Mo₃Se₃^-/polystyrene organogel exhibits significantly enhanced mechanical properties, with the improvement of 202.27% and 279.52% for tensile strength and elongation, respectively, compared with that of the pure organogel. The surface-modified Mo₃Se₃^- had a similar structure with a polymer matrix, and the properties of the polymer can be improved even with a small addition of Mo₃Se₃^-.