The available research does not allow specific relationships to be established between the applied enzymatic-mechanical treatment, the degree of polymerization, and the characteristics of the cellulose nanofibrils (CNFs) produced. This work aims to establish specific relationships between the intensity of enzymatic treatment, the degree of polymerization of the cellulose, the morphology of CNFs, and the tensile strength of the CNF films. It is determined that the decrease in the degree of polymerization plays an essential role in the fibrillation processes of the cell wall to produce CNFs and that there is a linear relationship between the degree of polymerization and the length of CNFs, which is independent of the type of enzyme, enzyme charge, and intensity of the applied mechanical treatment. In addition, it is determined that the percentage of the decrease in the degree of polymerization of CNFs due to mechanical treatment is irrespective of the applied enzyme charge. Finally, it is shown that the aspect ratio is a good indicator of the efficiency of the fibrillation process, and is directly related to the mechanical properties of CNF films.