The purpose of this study was to utilize cellulose from tea waste as nanocrystalline cellulose (NCC), which is used as a filler in poly(vinyl) alcohol (PVA) nanocomposites. To obtain the NCC, a chemical process was conducted in the form of alkali treatment, followed by bleaching and hydrolysis. Nanocomposites were formed by mixing PVA with various NCC suspensions. With chemical treatment, lignin and hemicellulose can be removed from the tea waste to obtain NCC. This can be seen in the functional groups of cellulose and the increase in crystallinity. The NCC had a mean diameter of 6.99 ± 0.50 nm. Furthermore, the addition of NCC to the PVA nanocomposite influenced the properties of the nanocomposites. This can be seen in the general increase in opacity value, thermal and mechanical properties, and crystallinity, as well as the decrease in the value of the swelling ratio after adding NCC. This study has revealed that NCC from tea waste can be used to improve the physicochemical properties of PVA film.