We herein report effects of morphology of PLLA and natural fiber on combination properties of biocomposites based on PLLA and ramie fibers. For this purpose, short ramie fiber (FIB), ramie fabric (FAB), PLLA film (FPLLA), and PLLA powder (PPLLA) were used to investigate the structure–property relationship of PLLA biocomposites with 30 wt% ramie fiber prepared by hot compression molding. It is revealed that mechanical properties of biocomposites are strongly dependent on the morphology of PLLA and FAB. DMA test shows that the improved storage modulus was due to the better dispersion of FIB. DSC and POM tests show that PLLA/FIB biocomposites have the highest spherulite growth rate. TGA test shows that char residue at high temperature is affected by the dispersion of PLLA and ramie fiber. SEM images exhibit the different interfacial adhesion character of FIB and FAB in the PLLA matrix after the ramie fiber treated with alkali and silane. PLLA/FAB biocomposites have not only better anti-dripping properties when burning but also better aging resistance in UV-irradiation hydrothermal aging, and which can be attributed to fiber bundle and laminated PLLA biocomposites structure. Copyright © 2010 John Wiley & Sons, Ltd.