Effects of additives with isocyanate group such as LDI and LTI on the mechanical properties of PLLA were investigated. It was found that bending properties of PLLA effectively increase due to addition of these additives. Fracture property of PLLA is also dramatically improved by adding 2phr of LDI and LTI. Isocyanate group of LDI and LTI and hydroxyl group of PLLA are chemically reacted and as a result, farm entangled structures are created. This kind of micro-structural modification is thought to be the primary mechanism of the improvement of the macro-mechanical properties.