<p>Phyllosilicate clay minerals are layered materials with dozens of unique morphologies (including nanoplaty, nanotubular, and nanofibrous shapes) and properties. These features make phyllosilicate nanoparticles suitable for application in many different industries, such as the paper industry, ceramic industry, cosmetic industry, pharmaceutical industry, etc. Since abundant resources are readily available, phyllosilicate minerals are particularly attractive because of their economic viability. Due to their high mechanical strength, thermal stability, and biocompatibility, phyllosilicate minerals also have numerous exciting potential applications in polymer nanocomposites. The goal of the research reported in this paper was to examine the potential application of these phyllosilicate nanoparticles in solid polymer electrolytes (SPEs) for lithium batteries. Four different phyllosilicate minerals were selected, including kaolinite (nanoplates), halloysite (nanotubes), montmorillonite (nanoplates/nanoparticles), and sepiolite (nanofibers). The electrochemical properties of different phyllosilicate nanoparticle modified SPEs were studied, including their ionic conductivity, lithium ion transference numbers (t+), and electrochemical stability windows. In addition, battery performance tests were performed to further evaluate the effectiveness of the phyllosilicate modified SPEs. The results indicate that the phyllosilicate nanoparticles, particularly halloysite, provide enhanced electrochemical properties for SPEs, and stable cycling performance results were achieved for different battery systems. Therefore, a new opportunity has been identified in this paper for the use of natural phyllosilicate nanoparticles in the lithium battery industry.</p>