Both cellulose nanocrystals (CNCs) and cellulose nanofibrils (CNFs) are nanoscale cellulose fibers that have shown reinforcing effects in polymer nanocomposites. CNCs and CNFs are different in shape, size and composition. This study systematically compared their morphologies, crystalline structure, dispersion properties in polyethylene oxide (PEO) matrix, interactions with matrix, and the resulting reinforcing effects on the matrix polymer. Transparent PEO/CNC and PEO/CNF nanocomposites comprising up to 10 wt % nanofibers were obtained via solution casting. Scanning electron microscopy (SEM), wide-angle X-ray diffraction (WXRD), transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR), dynamic mechanical analyzer (DMA), and tensile testing were used to examine the above-mentioned properties of nanocellulose fibers and composites. At the same nanocellulose concentration, CNFs led to higher strength and modulus than did CNCs due to CNFs' larger aspect ratio and fiber entanglement, but lower strain-at-failure because of their relatively large fiber agglomerates. The Halpin-Kardos and Ouali models were used to simulate the modulus of the composites and good agreements were found between the predicted and experimental values. This type of systematic comparative study can help to develop the criteria for selecting proper nanocellulose as a biobased nano-reinforcement material in polymer nanocomposites.