Tailoring the interconversion of electrical energy and chemical energy at the interface of solids and electrolytes stands as one of the preeminent challenges for next-generation energy technologies. Efficient electrochemical processes would enable electrical energy derived from renewable sources to be stored in chemical bonds for use in periods of low energy production. Electrochemical schemes for energy storage are exemplified in batteries, in which metal ions are inserted into a host lattice by intercalation. The basic science problem here lies in crafting and controlling complex surfaces to direct electron transfer across a solid–liquid interface reversibly and with a low energy barrier. These electronic and chemical demands are stringent, requiring a deep understanding of the fundamental factors that underpin interfacial electron transfer and chemical reactivity as well as the capability to finely manipulate the physicochemical properties of solids to bring about the desired interfacial chemistry. This talk will focus on recent work to manipulate and study the intercalation of lithium ions into two-dimensional (2D) heterostructures. I will also offer a brief outlook for exploiting 2D heterostructures to control other interfacial chemistries of relevance to energy storage in fuels, like the conversion of abundant, low energy materials like water, N2, and carbon dioxide into important industrial chemicals like H2, ammonia, and hydrocarbons.