The　development　of　porous　solid　adsorbents　for　selective　adsorption　and　separation　of　SO2has　attracted　much　attention　recently.　Herein,　we　design　porous　organic　polymers　(POPs)　decorated　with　pyridine　ligands　as　building　units　(POP-Py)　through　a　radical　polymerization　of　the　2,5-divinylpyridine　(v-Py)　monomer.　Due　to　its　high　BET　surface　area,　nanoporosity,　and　excellent　stability,　the　prepared　POP-Py　can　be　used　for　reversible　adsorption　and　efficient　separation　of　SO2.　The　POP-Py　possesses　a　SO2capacity　of　10.8　mmol　g-1at　298　K　and　1.0　bar,　which　can　be　well　retained　after　6　recycles,　showing　an　excellent　reversible　adsorption　capacity.　The　POP-Py　also　shows　superior　separation　performance　for　SO2from　a　ternary　SO2/CO2/N2mixture　(0.17/15/84.83v%),　giving　a　breakthrough　time　and　a　saturated　SO2capacity　at　178　min　g-1and　0.4　mmol　g-1.　The　retention　time　was　well　maintained　even　under　high　moisture　conditions,　confirming　its　superior　water　resistance.　Furthermore,　when　other　vinyl-functionalized　organic　ligand　monomers　(bipyridine,　pyrimidine,　and　pyrazine)　were　employed　for　radical　polymerization,　all　of　the　resultant　porous　organic　ligand　polymers　(POP-BPy,　POP-PyI,　and　POP-PyA)　exhibited　superior　performance　for　reversible　adsorption　and　efficient　separation　of　SO2.　The　combined　features　of　reversible　adsorption,　efficient　separation,　and　water　resistance　are　important　for　the　industrial　applications　of　these　materials　as　SO2adsorbents.　©　2022　American　Chemical　Society.　All　rights　reserved.