This talk outlines our approach to search for high-capacity hydrides capable of achieving the hydrogen storage system targets set by the US Department of Energy for hydrogen-fueled vehicles. Our research covers a broad composition space including both lightweight intermetallic hydrides and complex hydrides. High storage capacity requires that major constituents of solid-state storage materials be selected from the lightest 15 elements. Known compounds among these elements number in the hundreds, with many more unknown compounds anticipated. In order to analyze these potential hydrogen storage materials efficiently and rapidly, we employ a streamlined approach. An intelligent downselection is performed first, using phase diagram analysis, density functional theory (DFT) based computer simulations, and storage system-level analysis. Phase diagram analysis using both experimental data and CALPHAD results helps us to identify the possible phases that form during sorption and desorption. Computational modeling of hydride formation enthalpies using DFT is used to guide our selection of candidate systems along with system-requirement considerations. The selected candidate systems are evaluated using a high-throughput methodology. A diffusion-multiple approach is employed to generate hundreds of lightweight compounds and solid-solution compositions. Thin films and solution-based combinatorial libraries are also created for complex hydrides. These compositions are then screened with time-of-flight secondary ion mass spectrometry (ToF-SIMS) and other tools. Examples of several systems will be shown to illustrate our methodology.