Nathalia Vieira Villar de Nunes, S. Nunes da Silva, Eduarda Vieira Silva, André Lamounier Caixeta, Chiara das Dores do Nascimento, Everton Granemann Souza, Amanda Dantas de Oliveira, André Luiz Missio
Expanded polystyrene (EPS) waste is a major environmental concern, yet practical routes to upgrade it into higher value-added materials remain limited. Here, post-consumer EPS was dissolved in ethyl acetate and solvent-cast into films containing cellulose nanocrystals (CNCs) and a sunflower oil. Three formulations were produced: F-EPS (100% EPS), F-EPS + CEL (80% EPS/20% CNC), and F-EPS + CEL + OIL (80% EPS/15% CNC/5% oil). CNC markedly enhanced optical shielding, reducing transmittance at 400 nm from ≈58% (F-EPS) to ≈18% (CNC containing films). All films remained hydrophobic, showed negligible water uptake, and exhibited low mass loss after 30 days of accelerated weathering (ΔM=1–3%). Tensile testing showed that F-EPS had the highest UTS and elongation at break (10.0 ± 0.6 MPa and 10.5 ± 0.4%), whereas adding cellulose increased the elastic modulus (249.5 ± 29.0 MPa to 358.4 ± 64.8 MPa) but reduced UTS and elongation (8.2 ± 0.2 MPa and 5.4 ± 2.5%). Oil addition led to a further reduction in UTS and elongation (6.2 ± 0.4 MPa and 3.6 ± 0.0%), while the modulus returned to a value statistically similar to neat F-EPS. FTIR and XRD confirmed preservation of the EPS chemical fingerprint and a predominantly amorphous structure (2θ≈20–30°). Overall, EPS + CNC + OIL films combine hydrophobicity, UV-screening, and elastic modulus similar to neat F-EPS, supporting their use as moisture-resistant, UV screening protective topcoats for non-food-contact paperboard packaging.