MIL-100(Fe)　and　MIL-68(Fe),　two　Fe-based　MOFs,　were　found　to　be　active　for　oxidative　condensation　between　alcohols　and　o-aminothiophenols　to　form　2-substituted　benzothiazoles　under　visible　light　irradiation　using　oxygen　(O2)　as　oxidant.　This　reaction　can　be　applied　to　a　wide　range　of　substrates　with　medium　to　high　yield.　Controlled　experiments　and　ESR　results　revealed　a　superoxide　radical　(O2-)-mediated　pathway,　which　is　derived　from　the　reduction　of　O2　by　photogenerated　Fe2+　on　Fe–O　clusters.　The　whole　multistep　reaction　is　limited　by　the　step　of　the　photo-oxidation　of　alcohols　to　aldehydes.　MIL-100(Fe)　showed　catalytic　performance　superior　to　that　of　MIL-68(Fe)　because　its　higher　concentration　of　long-lived　(μs　time　scale)　positive　holes　can　be　photogenerated　over　MIL-100(Fe),　in　contrast　to　MIL-68(Fe).　This　study　not　only　provides　an　economical,　sustainable,　and　thus　green　process　for　the　production　of　2-substituted　benzothiazoles,　but　also　illustrates　the　potential　of　using　transient　absorption　spectroscopy　as　an　important　tool　for　understanding　the　photophysics　of　MOFs,　which　are　believed　to　show　great　potential　as　multifunctional　catalysts　for　light-induced　organic　transformations.　©　2017　Elsevier　Inc.