Sustainable chemical conversion of untapped synthetic resources in the environment e.g., greenhouse gases (CO2, methane), nitrogen, and water, to decarbonized fuels and feedstocks, powered by renewable electricity, can close the anthropogenic carbon loop at meaningful scales.1- 3 However, the technological progress of these complex chemical transformations is stymied due to the lack of systematic materials design principles, poor understanding of the complex and branched reaction pathways that control efficiency and selectivity, and complexities associated with elementary electron/mass/heat transfers in the reaction environment.3-5 Nano, micro and mesoscale structural engineering of materials and inorganic interfaces can have profound effects on the correlated bulk and surface physicochemical properties for judicious tuning of the crucial performance descriptors and reaction pathways. In my talk, I will take a few specific examples from my research to build a perspective on how the rational design of solid-state materials through multiscale engineering can solve some key scientific challenges in these low temperature electrondriven pathways through mechanistic understanding of structure-activity correlations.6-15 Based on these findings and existing challenges, I will try to derive the future course of fundamental and applied research in the materials and reaction engineering space for emerging chemical conversion routes, to drive the transition towards a circular energy and carbon economy.