In all, this work exemplified how a modular approach could be exploited to generate highly effective catalytic systems. In particular, by using an amine-appended terephthalic acid linker to assemble Ni-based MONs, we have enhanced the catalytic activity of the resultant material to attain near 100% selectivity for the 2e -oxygen reduction reaction pathway to peroxide. Further, translating this catalyst onto a GDE-based reactor, partial current densities of 200 mA/cm 2 were reached while maintaining a high 85% FE. While there are still open questions regarding the exact identity of the active sites (e.g. defects, local coordination), the nature of the MON structural dynamics during catalysis, and the precise reaction mechanism on the MON surfaces, this study opens up promising avenues to pursue in the design and understanding of peroxideproducing electrosynthetic systems.