Objectives: Maxillofacial silicone is used to restore abnormalities due to congenital or acquired causes. However, the quality of silicone is far from ideal. This study was aimed at assessing the influence of the addition of cellulose nanofibers (CNFs; several nanometers wide and 2-5 micro m long) on the physical and mechanical characteristics of maxillofacial silicone elastomers. Methods: Two CNF weight percentages (0.5% and 1%) were tested, and 180 specimens were divided into one control and two experimental groups. Each group was subdivided into six subgroups. In each subgroup, ten specimens subjected to each of the following tests: tearing strength, Shore-A hardness, tensile strength, elongation percentage, surface roughness, and color stability. The samples were additionally analyzed with Fourier transform infrared spectroscopy (FTIR) and field emission scanning electronic microscopy (FESEM). Results: The 0.5% CNF group, compared with the control group, exhibited highly significantly greater tearing strength, elongation percentage, hardness Shore-A, and surface roughness, and substantially greater tensile strength. However, color stability did not significantly differ between groups. The 1% CNF group showed significantly greater Shore-A hardness, tear strength, color stability, and surface roughness, and insignificantly lower tensile strength and percentage elongating values, than the control group. FESEM imaging revealed good CNF dispersion. The FTIR spectra indicated that CNFs interacted with silicon through surface functional hydroxyl groups. Conclusion: Addition of 0.5 wt. % CNF to silicone elastomers increased the material’s mechanical tensile strength, tear strength, elongation percentage, and hardness as long as it stayed within the acceptable range for clinical use. Surface roughness increased in direct proportion to the amount of nanofibers added. Moreover, addition of 0.5 wt. % CNF to silicone polymers had insignificant effects on color stability.