All-solid-state batteries offer a pathway to safer and higher-energy-density energy storage, but their practical implementation remains limited by challenges associated with ion transport, interfacial instability, and electrode architecture. Our research focuses on understanding and overcoming these bottlenecks through the development of advanced solid electrolytes, engineered interfaces, and high-performance composite cathodes. We investigate sulfide, halide, and hybrid solid electrolyte systems, with particular emphasis on the role of microstructure, stack pressure, ionic percolation, and chemo-mechanical evolution during battery operation. By combining operando characterization, electrochemical analysis, and materials design, we establish the structure-property-performance relationships that govern cell performance and durability, enabling the development of practical solid-state batteries with high energy density and long cycle life.