In this work, two different strategies for the development of amaranth protein isolate (API)-based films were evaluated. In the first strategy, ultrathin films were produced through spin-coating nanolayering, and the effects of protein concentration in the spin coating solution, rotational speed, and number of layers deposited on the properties of the films were evaluated. In the second strategy, cellulose nanocrystals (CNCs) were incorporated through a casting methodology. The morphology, optical properties, and moisture affinity of the films (water contact angle, solubility, water content) were characterized. Both strategies resulted in homogeneous films with good optical properties, decreased hydrophilic character (as deduced from the contact angle measurements and solubility), and improved mechanical properties when compared with the neat API-films. However, both the processing method and film thickness influenced the final properties of the films, being the ones processed through spin coating more transparent, less hydrophilic, and less water-soluble. Incorporation of CNCs above 10% increased hydrophobicity, decreasing the water solubility of the API films and significantly enhancing material toughness.