Carbon microspheres (CMSs) were oxidized by a mixture of concentrated sulfuric and nitric acids, and modified by 4-(chloromethyl)phenyltrimethoxysilane to give reactive surface. Then, by adopting the surface molecular imprinting technique, dibenzothiophene (DBT) molecule-imprinted material MIP-DBT/CMSs was prepared with methacrylic acid as functional monomer and ethylene glycol dimethacrylate as crosslinking agent. The binding character of MIP-DBT/CMSs toward DBT was investigated with static method by gas chromatography, using fluorene and biphenyl as the reference substances which are similar to DBT in chemical structure to a certain extent. The effects of reaction time, temperature, and coupling agent concentration during silanization were investigated. The results show that the optimized conditions of silanization were 0.3g oxidized-CMSs, 5% of CMTMS, 80°C and 4h. On the basis of silanized-CMSs, MIP-DBT/CMSs was synthesized. The adsorption results show that MIP-DBT/CMSs possessed strong adsorption ability for DBT. The maximal adsorption amount reached up 88.83mg/g, in comparison with 44.51mg/g of the non-imprinted polymer. In addition, MIP-DBT/CMSs exhibited a good selective adsorption capacity for DBT than fluorene (19.86mg/g) and biphenyl (15.33mg/g). The adsorption behavior followed the pseudo second order kinetic model. And the Freundlich isotherm was found to describe well the equilibrium adsorption data.