Abstract: As a novel adsorptive desulfurization method for the preparation of adsorbents, molecular imprinting technology is used to create specific molecular recognition sites in polymers to identify sulfur-bearing template molecules. It is a green process with potential applications because of its characteristics of mild conditions, simple operation, low investment, low pollution, high selectivity, no effect on octane value, and the possible reuse of the as-obtained benzothiophene-like compounds as fine chemicals. Recently, inorganic materials including silica gel, TiO2, K2Ti4O9, and carbon microspheres have been used as supports to prepare surface molecularly imprinted polymers for adsorbing dibenzothiophene and benzothiophene. Recent advances in molecular imprinting technology for deep desulfurization are summarized with carbon microsphere surface molecular imprinting technology highlighted. The review provides experimental references and theoretical guidance for designing and preparing green desulfurization materials.