Poly(lactic acid) (PLA)/palygorskite (Paly) nanocomposites were prepared using the melt compounding technique. Paly modified by 3-aminopropyltriethoxysilane (APTES) and vinyltrimethoxysilane (VTMS) was used as nanofiller for PLA with concentrations in the 1–7 wt% range. It has been found that the functionalization allows a covalent bond between the hydroxyl groups of the Paly and the PLA matrix, evidenced by the improvement in mechanical properties. Paly modification with VTMS has better properties compared with Pale modification with APTES. This indicates a better adhesion between the Paly-VTMS and PLA matrix, and a good dispersion of the nanofiller in the polymer matrix.