The efficient removal of H2S is necessary for clean production and energy safety. However, industrial gases are usually accompanied by CO2 significantly affecting desulfurization effects. Hence, novel imprinted adsorbents (PMo12@UiO-66@H2S-MIP-CDs) were synthesized through surface imprinting technology using cyclodextrins (CDs) as molecular scaffolds and UiO-66 modified by phosphomolybdic acid (PMo12@UiO-66) as a support. Wherein, PMo12@UiO-66@H2S-MIP-β-CD was determined as the optimal adsorbent since β-CD with low solubility is prone to keep its inherent cavity to promote dispersion of imprinted polymers and enrich internal pore channels. H2S capacity of PMo12@UiO-66@H2S-MIP-β-CD (31.67 mg/g) was about 2.4 and 1.7 times that of PMo12@UiO-66 and PMo12@UiO-66@H2S-MIPs, respectively, revealing the remarkable contribution of β-CD as a molecular scaffold to improve desulfurization. The results showed that PMo12@UiO-66@H2S-MIP-β-CD can maintain stable desulfurization efficiency regardless of the presence of CO2 or moisture, and O2 can strengthen the redox reaction between H2S and PMo12 accompanied by the increased reduction degree of Mo6+ in PMo12. After five adsorption-regeneration cycles, PMo12@UiO-66@H2S-MIP-β-CD still exhibited ideal removal efficiency. The excellent desulfurization performance is mainly ascribed to the selective adsorption role of H2S-MIP-β-CD and oxidative removal ability of PMo12. This work provides a valuable reference for the directional design of high-capacity functional adsorbents for room-temperature desulfurization.