Designing　frustrated　Lewis　pair　(FLP)-structured　photocatalysts　is　a　new　challenge　in　catalysis.　In　particular,　the　relationship　between　the　active　sites　and　photocatalytic　charge　transport　mechanism　over　FLP-structured　photocatalysts　is　still　ill-defined.　In　this　study,　a　novel　perylene-3,4,9,10-tetracarboxylic　diimide/UiO-66(Ti/Zr)-NH2　(denoted　as　PDI/TUZr)　photocatalyst　is　successfully　constructed　using　an　ammoniation　process.　The　PDI/TUZr　heterojunction　is　equipped　with　a　unique　＇Zr/Ti　SBUs-ligand-PDI＇　FLP　structure　and　exhibits　remarkable　catalytic　FLP　properties.　In　this　＇Zr/Ti　SBUs-ligand-PDI＇　structure,　the　Zr/Ti　bimetal　centers　and　PDI　serve　as　Lewis　acid　and　base　sites,　respectively,　and　the　C-N　chemical　bond　provides　a　channel　for　electron　transmission,　and　a　bimetallic　system　facilitates　electron　transfer　from　excited　ligand　to　Zr/Ti-SBUs　nodes.　These　superior　microstructural　designs　cooperate　to　promote　substrate　activation　for　photocatalytic　antibacterial　reactions.　Accordingly,　2.2-fold　enhancement　is　achieved　in　visible　photocatalytic　antibacterial　activity　on　Staphylococcus　aureus　for　4%PDI/0.2TUZr　composite　compared　with　unadorned　UZr.　This　study　provides　insights　into　the　formation　and　carrier　transfer　behaviors　of　solid　FLP　on　MOFs　and　illustrates　a　rational　strategy　for　the　construction　of　highly　efficient　photocatalysts.　©　2023　The　Royal　Society　of　Chemistry.