Lithium (Li), a key element in batteries for electric cars and other devices, has experienced a major demand surge in the past decade. While the primary source of lithium is from salt lakes, lithium-containing ores, and clay sources are widely distributed in the US and offer a potential alternative source for this important element. The challenge of using lithium found in clays and ores is separating the element from the complex sample, a process that is, in part, limited by the low reactivity of the aluminosilicate host structure. Current separation methods for lithium from ores or clay require high energy and/or chemical consumption needs. The objectives of this research are to develop a sustainable, electrochemical-facilitated leaching method to extract lithium from ores and clay. This research has the potential to contribute to the US critical mineral security, reduce reliance on lithium imports, and strengthen the scientific leadership of the US in the clean energy sector.