In general noble metals, transition metal-based materials, and carbon nanostructures have emerged as promising H2O2 selective catalysts with each possessing their advantages and drawbacks. One recurrent theme is the importance of identifying of the most active catalytic motifs within catalysts that possess a wide variety of surface terminations and possible active sites. An emerging class of materials beginning to find unique uses in electrochemical systems is organic/inorganic hybris systems such as metal-organic frameworks (MOFs), covalent-organic frameworks (COFs) and their derivatives. A particular advantage that they hold is their molecularly well-defined catalytic sites and modular structure that could enable the extraction of discreet structure-activity relationships. As such, only few metal-organic structures have been applied for H2O2 synthesis. In this work, we build on these previous studies and study the effects of linker identity on Ni-based metal-organic nanosheets (MONs). We construct MONs using terephthalic acid and several derivatives and characterize the resulting materials' physical and electronic structure with an array of techniques (Fig. ). We show how subtle differences in the Ni electronic structure conferred through changes in linker identity led to significant changes in H2O2 selectivity, with the Ni-Amine-MON exhibiting near 100% Faradaic efficiency (FE) towards H2O2. Finally, we translate the catalyst from a conventional 3-electrode setup to a gasdiffusion electrode (GDE) -based reactor and attain industrially-relevant H2O2 partial current densities of 200 mA/cm 2 while keeping an 85% FE for H2O2.