Composites were investigated regarding the comparison of multi-walled carbon nanotubes (MWCNTs) with exfoliated graphene(EG) in poly(L-lactic acid) (PLLA) and the effect of silane-treated carbon nanofillers on properties of PLLA composites. Solution blending method was used to prepare PLLA composites at a filler content of 0.5 wt %. Fourier transform infrared spectroscopy and X-ray photoelectron spectra results indicated the attachment of silane molecules on the surface of these nanofillers. It was found that the addition of these nanofillers greatly enhanced the mechanical, thermomechanical, and crystallization behaviors of PLLA due to the heterogeneous nucleation effect. Moreover, the silane-treated fillers further enhanced the breaking elongation moderately (although the materials are still brittle), modulus and thermal property of the nanocomposites, without sacrificing the tensile strength, compared with the pristine nanocomposites. On the other hand, composites reinforced with MWCNTs and EG perform almost the same mechanical property. And EG outperformed MWCNTs in thermomechanical properties of composites when being used as the reinforcement of PLLA. Conversely, composites reinforced with MWCNTs showed better crystallization properties than those reinforced with EG. Interestingly, no significant changes were observed for the crystallization properties of PLLA composites when MWCNTs and EG had been treated by silane coupling agent.