| Summary: | The present study focuses on the preparation and characterization of poly(3-hydroxybutyrate-<i>co</i>-3-hydroxyvalerate) (PHBV) films that were reinforced with cellulose microstructures to obtain new green composite materials for sustainable food packaging applications. The atomization of suspensions of microfibrillated cellulose (MFC) successfully allowed the formation of ultrathin cellulose structures of nearly 3 µm that were, thereafter, melt-mixed at 2.5, 5, and 10 wt % with PHBV and subsequently processed into films by thermo-compression. The most optimal results were attained for the intermediate MFC content of 5 wt %, however, the cellulose microstructures showed a low interfacial adhesion with the biopolyester matrix. Thus, two reactive compatibilizers were explored in order to improve the properties of the green composites, namely the multi-functional epoxy-based styrene-acrylic oligomer (ESAO) and the combination of triglycidyl isocyanurate (TGIC) with dicumyl peroxide (DCP). The chemical, optical, morphological, thermal, mechanical, and barrier properties against water and aroma vapors and oxygen were analyzed in order to determine the potential application of these green composite films in food packaging. The results showed that the incorporation of MFC yielded contact transparent films, whereas the reactive extrusion with TGIC and DCP led to green composites with enhanced thermal stability, mechanical strength and ductility, and barrier performance to aroma vapor and oxygen. In particular, this compatibilized green composite film was thermally stable up to ~280 °C, whereas it showed an elastic modulus (E) of above 3 GPa and a deformation at break (ɛ<sub>b</sub>) of 1.4%. Moreover, compared with neat PHBV, its barrier performance to limonene vapor and oxygen was nearly improved by nine and two times, respectively.
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