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Summary: With an increasing global emphasis on renewable energy, electrosynthetic technologies stand to play a substantial role in generating the fuels and chemicals that power today’s society. While directions such as water electrolysis and CO2 directions have been heavily researched in the last decade, the scope of electrosynthesis can be greatly expanded to cover the full range of chemical targets that serve as building blocks for materials, pharmaceuticals, fertilizers, and more. To this end, the main challenges lie in the discovery of novel reaction routes and innovative catalytic systems that circumvent conventional limitations of electrocatalysis. Against this backdrop, this perspective will focus on the use of emerging methodologies to pioneer new electrosynthetic reaction systems. In this work, strategies of environmental control, phase change materials, reactant-selective membranes, and mediated approaches are discussed, before touching on the innovative spectroscopic approaches used to probe these systems and wrapping up with a forward-thinking outlook.