Ultrathin　2D　materials　possess　unique　properties　that　translate　to　enhanced　efficiency　as　electrocatalysts,　stimulating　research　toward　methodologies　that　support　their　preparation.　Herein,　a　two-step　strategy　is　reported　that　involves　the　preparation　of　the　new　boron　imidazolate　framework　(BIF-73)　which　is　subsequently　utilized　as　a　precursor　to　yield　the　crystalline　2D　nanosheet　material　(Fe@BIF-73-NS)　via　post-synthetic　modification.　This　new　electrocatalytic　material　stabilizes　ultra-small　(Fe2O3)　fragments　resulting　in　an　excellent　electrocatalytic　performance　for　the　oxygen　evolution　reaction　(OER:　lower　overpotential　with　291　mV　at　the　current　density　of　10　mA　cm−2)　and　carbon　dioxide　reduction　reaction　(faradaic　efficiency　of　CO　reaching　88.6%　at　−1.8　V　vs　Ag/AgCl)　without　the　need　for　noble　metals.　Additionally,　theoretical　calculations　and　microscopy　reveal　that　the　superior　OER　performance　can　be　attributed　to　the　increased　exposure　of　binding　sites　within　the　material　to　which　the　catalytically　active　Fe3+　centers　are　bound　through　a　post-synthetic　modification　procedure.　A　red-shift　of　the　Fermi　level　around　the　valence　band　is　observed　and　is　proposed　to　be　a　result　of　the　aforementioned　interactions.　This　work　opens　an　avenue　toward　the　development　of　2D　functional　metal　organic　framework　nanosheets　for　energy　conversion　applications.　©　2020　WILEY-VCH　Verlag　GmbH　&　Co.　KGaA,　Weinheim