Computational screening techniques have been found to be an effective alternative to the trial and error of experimentation for discovery of new materials. With increased interest in development of advanced electrical energy storage systems, it is essential to find new electrolytes that function effectively. This Perspective reviews various methods for screening electrolytes and then describes a hierarchical computational scheme to screen multiple properties of advanced electrical energy storage electrolytes using highthroughput quantum chemical calculations. The approach effectively down-selects a large pool of candidates based on successive property evaluation. As an example, results of screening are presented for redox potentials, solvation energies, and structural changes of ∼1400 organic molecules for nonaqueous redox flow batteries. Importantly, on the basis of high-throughput screening, in silico design of suitable candidate molecules for synthesis and electrochemical testing can be achieved. We anticipate that the computational approach described in this Perspective coupled with experimentation will have a significant role to play in the discovery of materials for future energy needs.