High lignin-containing cellulose nanocrystals (HLCNCs) were successfully isolated from hydrothermally treated aspen fibers and freeze-dried and compounded with poly (lactic acid) (PLA) by extrusion and injection molding. As a comparison, PLA composites containing commercial lignin-coated CNCs (BLCNCs) were also produced. HLCNCs showed higher crystallinity, larger surface area, lower degree of agglomeration, and more hydrophobic surfaces compared to BLCNCs, as characterized by electron microscopy, surface area measurements, thermal analysis, spectroscopy and water contact angle measurements. The effect of lignin and CNC morphology on the mechanical, thermal and viscoelastic properties and CNCs/polymer interfacial adhesion of nanocomposites was investigated with tensile test, DSC and DMA. Compared to neat PLA, the Young's modulus, elongation to break, and toughness of PLA/2%HLCNCs were improved by 14, 77, and 30%, respectively. HLCNCs and BLCNCs act as nucleating fillers, increasing the degree of crystallinity (chi(c)) of PLA in nanocomposites. The presence of lignin nanoparticles in the HLCNC increased the compatibility/adhesion between CNCs and polymer matrix which increased the storage modulus. Published by Elsevier Ltd.