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Atomically dispersed metals maximize the number of catalytic sites and enhance their activity. However, their challenging synthesis and characterization strongly complicates their optimization. Here, the aim is to demonstrate that tuning the electronic environment of atomically dispersed metal catalysts through the modification of their edge coordination is an effective strategy to maximize their performance. This article focuses on optimizing nickel-based electrocatalysts toward alcohol electrooxidation in alkaline solution. A new organic framework with atomically dispersed nickel is first developed. The coordination environment of nickel within this framework is modified through the addition of carbonyl (CO) groups. The authors then demonstrate that such nickel-based organic frameworks, combined with carbon nanotubes, exhibit outstanding catalytic activity and durability toward the oxidation of methanol (CHOH), ethanol (CHCHOH), and benzyl alcohol (CHCHOH); the smaller molecule exhibits higher catalytic performance. These outstanding electrocatalytic activities for alcohol electrooxidation are attributed to the presence of the carbonyl group in the ligand chemical environment, which enhances the adsorption for alcohol, as revealed by density functional theory calculations. The work not only introduces a new atomically dispersed Ni-based catalyst, but also demonstrates a new strategy for designing and engineering high-performance catalysts through the tuning of their chemical environment. ; ICN2 is supported by the Severo Ochoa program from Spanish MINECO (Grant No. SEV-2017-0706) and is funded by the CERCA Programme /Generalitat de Catalunya. Part of the present work has been performed in the framework of Universitat Autònoma de Barcelona Materials Science Ph.D. program. Z.L. acknowledges funding from MINECO SO-FPT Ph.D. grant (SEV-2013-0295-17-1). This project has received funding from the European Union's Horizon 2020 research and innovation program under grant agreement No 823717-ESTEEM3. The present work is supported by the European Regional Development Fund and by the Spanish MINECO through the projects ENE2016-77798-C4-3-R, ENE2017-85087-C3, and project NANOGEN (PID2020-116093RB-C43). X.W. and T.Z. thank the China Scholarship Council for the scholarship support. P. Tang acknowledges the Humboldt Research Fellowship. Authors acknowledge funding from Generalitat de Catalunya 2017SGR327 and 2017SGR1246. L.L. acknowledges the support from Natural Sciences and Engineering Research Council of Canada (NSERC, DG RGPIN-2020-06675). J.L. is a Serra Húnter Fellow and is grateful to MICINN/FEDER RTI2018-093996-B-C31, GC 2017 SGR 128, and to ICREA Academia program.