In　spite　of　significant　developments　are　accomplished　in　the　exploration　of　H2　and　O2　evolution　upon　water　electrolysis/photolysis,　this　remains　a　challenge　to　design　and　develop　ideal　catalytic　systems　for　this　reaction　and　to　isolate　H2　from　H2-O2　mixture　with　membranes.　Herein,　a　series　of　ZIF-67-supported　transition　metal　nanoparticles　(TMNPs/ZIF-67),　including　Pt,　Ir,　Pd,　Rh,　Au　and　Ag,　via　immobilization　of　ultrafine　TMNPs　at　the　surface　of　ZIF-67,　have　been　designed　and　developed　for　the　selective　H2　generation　from　NH3BH3　hydrolysis　and　O2　evolution　upon　H2O2　decomposition.　In　particular,　the　optimized　nanocatalyst　Pt/ZIF-67　presents　the　super-high　catalytic　property　in　the　both　H2　evolution　upon　NH3BH3　hydrolysis　(689　mol(H2)·molPt-1·min−1)　and　O2　evolution　upon　H2O2　decomposition　(979　mol(O2)·molPt-1·min−1)　at　30　°C.　Importantly,　the　selective　“on–off”　control　for　demand-based　H2　generation　from　NH3BH3　hydrolysis　was　successfully　realized　by　Zn2+/EDTA-2Na　system.　This　highly　efficient　Pt/ZIF-67　proposed　a　new　method　for　the　promising　potential　application　of　ammonia　borane　and　hydrogen　peroxide　as　an　economic　and　safe　H2　resp.　O2　carrier　for　fuel　cell.　©　2023　Elsevier　Ltd