The Mercer Clay bed in central Pennsylvania has produced feedstocks for the refractory industry in the USA and has also been investigated as a source of alumina and lithium. Developments in global markets for these commodities, as well as rare earth elements, have led to their classification as critical minerals in the USA, in turn renewing production opportunities for the Mercer Clay resource. The work reported here includes a review of the clay types and minerals involved, as well as past mineral processing and extractive metallurgy test work, and reports new research results from renewed investigation of the deposit as a polymetallic resource. This renewed work has found lithium contents that exceed 1,000 ppm, lying directly below the overlying Mercer coal, where the alumina content ranged from 32 to 34 wt%. Total rare earth concentrations were somewhat lower than have been found elsewhere in the region, and the highest contents were also found to be stratigraphically close to the coal. Further work is required to establish the mineral hosts for lithium and rare earths and to define the extent of enriched alumina, lithium, and rare earth concentrations.