Recently, hybrid fillers have been widely used to improve the properties of biopolymers. The synergistic effects of the hybrid fillers can have a positive impact on biopolymers, including thermoplastic corn starch film (TPCS). In this communication, we highlight the effectiveness of hybrid fillers in inhibiting the aging process of TPCS. The TPCS, thermoplastic corn starch composite films (TPCS-C), and hybrid thermoplastic corn starch composite film (TPCS-HC) were stored for 3 months to study the effect of hybrid filler on the starch retrogradation. TPCS-C and TPCS-HC were prepared by casting method with 5 wt% of fillers: nanocellulose (NC) and bentonite (BT). The alteration of the mechanical properties, aging behavior, and crystalline structure of the films were analyzed through the tensile test, Fourier transform infrared (FTIR), X-ray diffraction (XRD), differential scanning calorimetry (DSC), and water absorption analysis. The obtained data were correlated to each other to analyze the retrogradation of the TPCS, which is the main factor that contributes to the aging process of the biopolymer. Results signify that incorporating the hybrid filler (NC + BT) in the TPCS/4BT1NC films has effectively prevented retrogradation of the starch molecules after being stored for 3 months. On the contrary, the virgin TPCS film showed the highest degree of retrogradation resulting in a significant decrement in the film’s flexibility. These findings proved the capability of the green hybrid filler in inhibiting the aging of the TPCS.

This study focuses on investigating the effect of hybrid nanofillers on the hydration characteristics and soil biodegradability of the thermoplastic corn starch (TPCS) hybrid nanofiller biocomposite (TPCS-HB) films. The data were benchmarked with that of the pure TPCS and TPCS single nanofiller biocomposite (TPCS-SB) as control films. The water absorption properties of TPCS, TPCS-SB, and TPCS-HB films were analyzed and fitted with the standard Guggenheim–Anderson–de Boer equation to study the water activity of the films. Besides, the water permeability test, water vapor permeability, and soil biodegradability of the films were also studied and correlated with the films’ surface morphology. The results indicated that the TPCS-HB films possess excellent hydration resistance and comparable biodegradable rate with the TPCS-SB films. The optimal water resistance properties were achieved when the optimal ratio of nanobentonite/nanocellulose (4:1) was incorporated into the TPCS matrix. The outcomes of this study provide an innovative idea and new insights that, by using natural and hybrid nanofillers, the hydrophobicity of the TPCS films could be enhanced. TPCS-HB films show great potential to be developed into a fully green biodegradable TPCS biocomposite film, especially for single-use plastic applications.