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Quinoa starch nanocrystals (QSNCs), obtained by acid hydrolysis, were used as a reinforcing filler in cassava starch films. The influence of QSNC concentrations (0, 2.5, 5.0, 7.5 and 10%, w/w) on the film’s physical and surface properties was investigated. QSNCs exhibited conical and parallelepiped shapes. An increase of the QSNC concentration, from 0 to 5%, improved the film’s tensile strength from 6.5 to 16.5 MPa, but at 7.5%, it decreased to 11.85 MPa. Adequate exfoliation of QSNCs in the starch matrix also decreased the water vapor permeability (~17%) up to a 5% concentration. At 5.0% and 7.5% concentrations, the films increased in roughness, water contact angle, and opacity, whereas the brightness decreased. Furthermore, at these concentrations, the film’s hydrophilic nature changed (water contact angle values of >65°). The SNC addition increased the film opacity without causing major changes in color. Other film properties, such as thickness, moisture content and solubility, were not affected by the QSNC concentration. The DSC (differential scanning calorimetry) results indicated that greater QSNC concentrations increased the second glass transition temperature (related to the biopolymer-rich phase) and the melting enthalpy. However, the film’s thermal stability was not altered by the QSNC addition. These findings contribute to overcoming the starch-based films’ limitations through the development of nanocomposite materials for future food packaging applications.