We undertook this study to understand reinforcement mechanism of short cellulose nanocrystals (CNCs) and long cellulose nanofibrils (CNFs) as compatibility agents for improving the interfacial miscibility of poly(vinyl alcohol) (PVA) and poly(ethylene oxide) (PEO) blends. The effects of the two cellulose nanofibers on the morphological, mechanical, and thermal properties of the polymer blends were compared systematically. The light transparency, scanning electron microscopy, and Fourier transform infrared results show that nanocellulose between PVA and PEO eliminated the negative effects generated by the immiscible interface through increased hydrogen bonding. Thermogravimetric analysis and differential scanning calorimetry results show that crystalline region reorganization around the interface facilitated the shift of the polymer blends from multiple phases to a homogeneous phase. According to the Halpin‐Kardos and Quali models, we assumed that the potential for repairing the immiscible interface would have a larger effect than the potential of reinforcement. At the same concentration, polymer blends with CNCs showed greater light transparency, strength, modulus, and crystal structure than with those with CNFs. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018, 135, 45896.