Poly(L-lactide) (PLLA)-based biocomposites incorporated with different amounts of chitosan oligosaccharide (COS) were developed through solvent-casting method. Then, the physical-chemical properties, surface morphology, hydrophilicity, water uptake, biodegradability, and biocompatibility of the COS/PLLA composites were investigated. Fourier transform infrared and X-ray diffraction results showed that strong hydrogen-bonding interactions were presented between the COS and PLLA components. Scanning electron microscope and atomic force microscope images revealed that COS physically attached on the PLLA surface enhanced the formation of the surface seepage network, which led to the improvement of the surface biological features. A gradual rise in the level of hydrophilicity, water uptake, and degradation rate in phosphate buffered saline solution were found on increasing COS content in the COS/PLLA composites, which may provide effective support for cell adhesion and proliferation. Further, the results of cell experiments also suggested that the COS/PLLA composites had better cytocompatibility compared with PLLA. Thus, the COS/PLLA composites may have the great potential to be used for soft and bone tissue repair.