A　series　of　zirconium　polyphenolate-decorated-(metallo)porphyrin　metal–organic　frameworks　(MOFs),　ZrPP-n　(n　=　1,　2),　featuring　infinite　ZrIV-oxo　chains　linked　via　polyphenolate　groups　on　four　peripheries　of　eclipse-arranged　porphyrin　macrocycles,　are　successfully　constructed　through　a　top–down　process　from　simulation　to　synthesis.　These　are　the　unusual　examples　of　Zr-MOFs　(or　MOFs　in　general)　based　on　phenolic　porphyrins,　instead　of　commonly　known　carboxylate-based　types.　Representative　ZrPP-1　not　only　exhibits　strong　acid　resistance　(pH　=　1,　HCl)　but　also　remains　intact　even　when　immersed　in　saturated　NaOH　solution　(≈20　m),　an　exceptionally　large　range　of　pH　resistance　among　MOFs.　The　metallation　at　the　porphyrin　core　gives　rise　to　materials　with　enhanced　sorption　and　catalytic　properties.　In　particular,　ZrPP-1-Co,　with　precise　and　uniform　distribution　of　active　centers,　exhibits　not　only　high　CO2　trapping　capability　(≈90　cm3　g−1　at　1　atm,　273　K,　among　the　highest　in　Zr-MOFs)　but　also　high　photocatalytic　activity　for　reduction　of　CO2　into　CO　(≈14　mmol　g−1　h−1)　and　high　selectivity　over　CH4　(＞96.4%)　without　any　cocatalyst　under　visible-light　irradiation　(λ　＞　420　nm).　Given　the　strong　chemical　resistance　under　extreme　alkali　conditions,　these　catalysts　can　be　recycled　without　appreciable　loss　of　activity.　The　possible　mechanism　for　photocatalytic　reduction　of　CO2-to-CO　over　ZrPP-1-Co　is　also　proposed.　©　2017　WILEY-VCH　Verlag　GmbH　&　Co.　KGaA,　Weinheim