A new method was attempted to improve the interaction between poly(L-lactide) (PLLA) with a commercially available organoclay, Cloisite 25A (C25A), which was functionalized with (glycidoxypropyl)trimethoxysilane to introduce epoxy groups, and is referred to as twice-functionalized organoclay (TFC). Tethering PLLA molecules to the epoxy groups on the surface of the TFC was attempted by melt compounding. X-Ray diffraction and transmission electron microscopy images showed that fully exfoliated PLLA/TFC nanocomposites were prepared sucessfully.