Electrochemical hydrogenation reactions offer a green and sustainable production pathway for both bulk and fine chemicals employed in the modern chemical industry. However, optimizing such systems can be tremendously challenging due to the number of variables that potentially influence the overall performance. The tailored and scalable electrode fabrication via catalytic inks can be especially difficult due to the complex interplay of material and process variables during the formulation of the inks and their deposition on suitable substrates. As a result, the significance of each variable must be systematically investigated to reveal the high‐impact and low‐impact variables, enabling rapid progression towards finding optimal conditions and parameters. In this work, we present an adaptable, coherent workflow to proficiently optimize electrode fabrication for electrochemical hydrogenation reactions with well‐adjustable experimental effort. Using the hydrogenation of phenylacetylene as a model reaction in a scalable zero‐gap reactor, we demonstrate the influence of deposition techniques, substrates, and catalyst loadings as well as the interactions of binders and additives on the electrochemical performance. Future works can greatly benefit from this coherent workflow as it enables direct comparability between datasets and functional, multidimensional optimization, hastening the rate at which new material systems are understood, reach maturity, and become industrially relevant.