In　principle,　porous　physisorbents　are　attractive　candidates　for　the　removal　of　volatile　organic　compounds　such　as　benzene　by　virtue　of　their　low　energy　for　the　capture　and　release　of　this　pollutant.　Unfortunately,　many　physisorbents　exhibit　weak　sorbate–sorbent　interactions,　resulting　in　poor　selectivity　and　low　uptake　when　volatile　organic　compounds　are　present　at　trace　concentrations.　Herein,　we　report　that　a　family　of　double-walled　metal–dipyrazolate　frameworks,　BUT-53　to　BUT-58,　exhibit　benzene　uptakes　at　298　K　of　2.47–3.28　mmol　g−1　at　2BDP　=　1,4-di(1H-pyrazol-4-yl)benzene),　captures　trace　levels　of　benzene,　producing　an　air　stream　with　benzene　content　below　acceptable　limits.　Furthermore,　BUT-55　can　be　regenerated　with　mild　heating.　Insight　into　the　performance　of　BUT-55　comes　from　the　crystal　structure　of　the　benzene-loaded　phase　(C6H6@BUT-55)　and　density　functional　theory　calculations,　which　reveal　that　C–H···X　interactions　drive　the　tight　binding　of　benzene.　Our　results　demonstrate　that　BUT-55　is　a　recyclable　physisorbent　that　exhibits　high　affinity　and　adsorption　capacity　towards　benzene,　making　it　a　candidate　for　environmental　remediation　of　benzene-contaminated　gas　mixtures.　©　2022,　The　Author(s).