Surface grafting of crystalline and ultrafine cellulose nanofibrils with poly(ethylene glycol) (PEG) chains via ionic bonds was achieved by a simple ion-exchange treatment. The PEG-grafted cellulose nanofibrils exhibited nanodispersibility in organic solvents such as chloroform, toluene, and tetrahydrofuran. Then, the PEG-grafted cellulose nanofibril/chloroform dispersion and poly(l-lactide) (PLLA)/chloroform solution were mixed, and the PEG-grafted cellulose nanofibril/PLLA composite films with various blend ratios were prepared by casting the mixtures on a plate and drying. The tensile strength, Young’s modulus, and work of fracture of the composite films were remarkably improved, despite low cellulose addition levels (<1 wt %). The hig...