The current research is intended to optimize the formulation of bionanocomposite films produced from polyvinyl alcohol by adding glycerol (4–8%) and cellulose nanocrystals extracted from pineapple crown leaf (3–7%). The interaction between the bionanocomposite films characteristic, such as thickness, tensile strength, and elongation are determined using a response surface methodology with a central composite design. To show the practical relevance of the prediction model, the optimized bionanocomposite film composition required additional validation. Adding glycerol at 4% and cellulose nanocrystal at 3.52% was determined to be the film’s optimum parameters. Improved mechanical properties with a low thickness value and high elongation were found in the enhanced film formulation. The findings showed that an optimized bionanocomposite film formulation based on polyvinyl alcohol with glycerol and cellulose nanocrystals from pineapple crown leaves provided good model validation and could be utilized optimally in the food packaging application.