In practical scenarios, destabilizing the physical attributes of natural polymers such as gelatin and starch occurs readily when exposed to specific moisture levels and heat. In this context, this work was carried out to assess the impact of PVA addition (up to 13 wt%) on the structure and physical properties of a 6:4 (w/w) gelatin/starch blend. The inclusion of PVA unfolded the molecular chains of gelatin and starch, thereby disrupting gelatin α-helices and impeding biopolymer crystallization. This facilitated hydrogen-bonding interaction between PVA and the two biopolymers, enhancing the stability of the molecular network structure. Rheological results indicate that composites (added with 4 % or 7 % PVA) with good compatibility exhibited excellent mechanical properties and deformation resistance. The addition of PVA elevated the gelling temperature (Tgel) of the composites from 41.31 °C to 80.33 °C; the tensile strength and elongation at break were increased from 2.89 MPa to 3.40 MPa and 341.62 % to 367.56 %, respectively; and the thermal stability was also apparently improved, signifying the effective enhancement of the physical properties of gelatin/starch-based composites and the broadening of their application scope. This work could provide insights into the development of biodegradable natural/synthetic polymer composites with application-beneficial characteristics.
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