This study successfully synthesizes CoAl-hexametaphosphate layered double hydroxide (HMP-LDH) via anion exchange. The application of HMP-LDH leads to substantial wear and friction reduction of 88% and 25%, respectively, outperforming the PAO-4 base oil. In-depth characterizations of tribofilms formed on wear scars and tracks were conducted using various techniques, including Raman, X-ray photoelectron spectroscopy, scanning transmission electron microscopy - energy dispersive X-ray spectroscopy, and cryo-electron energy loss spectroscopy. It was found that the predominant composition of the tribofilm consists of mixed oxide and phosphate species. Notably, metallic cobalt is observed near the tribofilm-steel interface. Nanoindentation and nanoscratch were performed on the HMP tribofilm. The relationship between the nanostructure and nanomechanical properties and their influence on friction and wear have been revealed.