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A series of high dielectric composite films based on low-cost and eco-friendly titanium dioxide (TiO
2
) and cellulose nanofibril (CNF) was prepared under a facile condition. The relative dielectric constants (ε
r
) and dielectric loss (
tan
δ
) were studied as the function of frequency and filler content. The ε
r
of CNF/TiO
2
composite film was 19.51 (at 1 kHz) with a relatively low dielectric loss. Compared with pure CNF films (ε
r
= 6.92 at 1 kHz), the ε
r
of the composite film was improved about three times with the dielectric loss increased slightly. The effects of TiO
2
addition and hot-press treatment on microstructure, thermal stability, and dynamic mechanical properties of the composite films were also analyzed. It was found that the addition of TiO
2
particles reduces the cellulose–cellulose bonding so generates more pores in the films, which has significant impacts on both dielectric and physical strength properties.
Graphical abstract