An acid dye molecule surface-imprinted material was prepared successfully for the dye removal from water by using a novel molecular surface-imprinting technique. The cationic monomer acryloyloxyethyl trimethyl ammonium chloride (DAC) was used as functional monomer, and sunset yellow was used as a model compound of water-soluble acid dyes. In the aqueous solution, DAC molecules were combined around sunset yellow molecules via electrostatic interaction. The graft/cross-linking copolymerization of DAC and the crosslinker on SiO2 particles was initiated by a surface-initiating system of -NH2/S2O82-, resulting in the sunset yellow molecule surface-imprinted material MIP-PDAC/SiO2. MIP-PDAC/SiO2 possesses special recognition property for sunset yellow.