The dataset contains raw data supporting the article ‘Driving electrochemical organic hydrogenations on metal catalysts by tailoring hydrogen surface coverages’. This work presents a computationally guided design of electrochemical hydrogenation catalysts by optimizing hydrogen coverage density and binding strength on the electrode. It highlights the potential of tailoring the hydrogen coverage on electrode surfaces to rationally design non-precious metal electrocatalysts for efficient organic hydrogenation. The dataset is divided into five key parts: i) Organic Hydrogenation Assembly: Contains schematic representation of the organic hydrogenation system, ii) Electrocatalysis: Electrochemical characterisation of the electrocatalysts, including cyclic voltammetry, Faradaic efficiency, current density, conversion of reactant and yield of products, iii) Materials Characterisation: Physical characterisation of the metal electrocatalysts, iv) Computations: theoretical calculations of the surface hydrogen coverage and reaction mechanism, and v) Spectroscopy: proton NMR characterisation for the reaction mixture. For more details about experimental procedure, instrumentation, and data collection, see the manuscript.