Cassava bagasse, a high-fiber coproduct of cassava starch processing, was used to produce lignocellulose nanofibers (LCNF) to apply as reinforcement in cassava starch films. LCNF-reinforced cast starch films were evaluated for changes in structural, thermal and mechanical properties and compared with control films reinforced with commercial grade nanoclay (Nclay). Five different types of cassava starch cast-films were produced: no-reinforcement control, two LCNF-reinforced, and two Nclay-reinforced, each at 0.65 and 1.3% w w−1. The LCNF morphology showed the characteristic microscopic structure of lignocellulose nanofibers, with an aspect ratio > 85 and average diameter of 4.5 nm. All reinforced films were transparent and had a good distribution of the nanoparticles within. The opacity values reduced for the films with all nanoreinforcements, compared to control. The permeability to water vapor reduced with reinforcements, with lower values for the films tested with LCNF 0.65 and Nclay 1.3. Thermal stability improved with 1.3% of LCNF and both concentrations of Nclay. Tensile stress for films increased and elongation at break value decreased with both types of nanoreinforcements.