The　selective　removal　of　sulfur　dioxide　(SO2)　is　of　importance　for　the　desulfurization　and　purification　of　exhaust　gases,　but　it　is　still　challenging　to　design　adsorbents　with　high　capture　capacities　(particularly　at　low　partial　pressures)　and　great　cyclic　stability.　Herein,　a　facile　strategy　is　proposed　to　optimize　the　adsorption　performance　of　NaY　zeolites,　where　various　alcohol-terminated　compounds　(n-pentanol,　ethylene　glycol,　polyethylene　glycol)　with　different　molecular　structures　are　introduced　as　auxiliaries　to　facilitate　the　zeolite　nucleation　process　and　the　formation　of　microporous　structures.　These　alcohols　promote　the　crystallization　of　NaY,　increase　the　specific　surface　area　and　expand　the　microporosity　due　to　the　formation　of　micelles　during　synthesis.　Coupled　with　the　rise　of　surface　basic　sites,　the　chemisorption　and　physisorption　of　SO2　on　designed　zeolites　is　considerably　improved.　The　PEG-Y　sample　derived　from　polyethylene　glycol　gives　the　highest　dynamic　adsorption　of　SO2　(315　mg/g),　high-level　SO2　equilibrium　adsorption　(2.18　mmol/g)　under　exceptionally　low　pressure　(0.002　bar),　preferred　separation　performance　of　SO2　from　SO2/N2,　robust　stability　and　great　regenerability.　This　technique　can　be　further　employed　to　fabricate　analogous　adsorbents　for　other　gas　adsorption　and　separation　processes.