The global energy infrastructure is undergoing a seismic transformation towards sustainable and highly efficient technologies for energy conversion and storage, including fuel cells, electrolysis cells (for water or CO2), and modern batteries. Energy materials that are inexpensive, abundant, and environmentally benign while fulfilling exacting technology needs in terms of performance, durability, and longevity, are crucial enablers of this transition. Our program in theory, modeling, and simulation strives to increase fundamental understanding of vital electrochemical phenomena, support the development of tailor-made materials solutions and diagnostic approaches, and devise model-based tools for the evaluation and optimization of next-generation devices. To expedite this agenda, we make use of a broad inventory of tools, from quantum mechanical simulations to continuum modeling. Our research program offers ample interfaces for model evaluation by comparison to experiments, knowledge transfer to materials science laboratories, and testing and analytics of innovative materials in functional energy devices. The scientific program is complemented by the development of a Virtual Materials Intelligence platform.