Warm-season　O-3　pollution　has　been　increasingly　frequent　worldwide　in　the　past　few　years,　exposing　a　threat　to　human　health　as　well　as　the　natural　environment.　Here,　the　authors　showcase　a　stable　MOF　which　can　not　only　effectively　capture　various　airborne　VOCs,　but　decompose　trace　O-3　in　ambient　air.　Atmospheric　ozone　has　long　been　a　threat　to　human　health,　however,　rational　design　of　high-performance　O-3-decomposition　catalysts　remains　challenging.　Herein,　we　demonstrate　the　great　potential　of　a　series　of　isomorphous　bimetallic　MOFs　denoted　as　PCN-250(Fe2M)　(M　=　Co2+,　Ni2+,　Mn2+)　in　catalytic　O-3　decomposition.　Particularly,　PCN-250(Fe2Co)　showed　100%　O-3　removal　efficiency　for　a　continuous　air　flow　containing　1　ppm　O-3　over　a　wide　humidity　range　(0　-　80%　RH)　at　room　temperature.　Mechanism　studies　suggested　that　the　high　catalytic　performance　originated　from　the　introduction　of　open　Co(II)　sites　as　well　as　its　porous　structure.　Additionally,　at　low　pressures　around　10　Pa,　PCN-250(Fe2Co)　exhibited　high　adsorption　capacities　(89　-　241　mg　g(-1))　for　most　VOCs,　which　are　not　only　a　class　of　hazardous　air　pollutants　but　also　the　precursor　of　O-3.　This　work　opens　up　a　new　avenue　to　develop　advanced　air　purification　materials　for　O-3　and　VOCs　removal　in　one.