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Cellulose nanocrystals (CNCs) isolated from banana pseudostems fibers (BPF) of the Pacovan variety were used as fillers in a polyvinyl alcohol (PVOH) matrix to yield a nanocomposite. The fibers from the external fractions of the BPF were alkaline bleached and hydrolyzed under acidic conditions (H₂SO₄ 62% w/w, 70 min, 45 °C) to obtain CNCs with a length (L) of 135.0 ± 12.0 nm and a diameter (D) of 7.2 ± 1.9 nm to yield an aspect ratio (L/D) of 21.2. The CNCs were applied to PVOH films at different concentrations (0%, 1%, 3%, and 5% w/w, dry basis). With higher concentrations of CNCs, the water–vapor barrier of the films increased, while the optical properties changed very little. Increasing the concentration of the CNCs up to 3% significantly improved the mechanical properties of the nanocomposite.