Biopolymers, which are biodegradable and inherently functional, have high potential for specialized applications (e.g., disposable and transient systems and biomedical treatment). For this, it is important to create composite materials with precisely defined chain interactions and tailored properties. This work shows that for a chitosan–gelatin material, both glycerol and isosorbide are effective plasticizers, but isosorbide could additionally disrupt the polyelectrolyte complexation (PEC) between the two biopolymers, which greatly impacts the glass transition temperature (T_g), mechanical properties, and water absorption. While glycerol-plasticized samples without nanofiller or with graphene oxide (GO) showed minimal water uptake, the addition of isosorbide and/or montmorillonite (MMT) made the materials hydrolytically unstable, likely due to disrupted PEC. However, these samples showed an opposite trend in surface hydrophilicity, which means surface chemistry is controlled differently from chain structure. This work highlights different mechanisms that control the different properties of dual-biopolymer systems and provides an updated definition of biopolymer plasticization, and thus could provide important knowledge for the future design of biopolymer composite materials with tailored surface hydrophilicity, overall hygroscopicity, and mechanical properties that meet specific application needs.

This study successfully developed edible films with excellent mechanical strength and notable water resistance, utilizing curdlan (CL) as the primary matrix and incorporating various plasticizers, including glycerol (GLY), ethylene glycol (EG), propylene glycol (PRO), xylitol (XY), sorbitol (SOR), and polyethylene glycol (PEG). A comprehensive suite of analytical techniques, including Fourier transform infrared spectroscopy (FTIR), wide-angle X-ray diffraction (XRD), scanning electron microscopy (SEM), dynamic mechanical analysis (DMA), and tensile testing, were employed to evaluate the films’ structural and mechanical properties. After incorporating PEG, the water sensitivity increased slightly, with a contact angle (CA) of 97.6°, and a water solubility (WS) of 18.75%. The inclusion of plasticizers altered the crystalline structure of the CL matrix, smoothing and flattening the film surface while reducing hydrogen-bonding interactions. These structural changes led to a more uniform distribution of amorphous chain segments and a decrease in glass transition temperatures. Among the tested plasticizers, GLY exhibited the highest compatibility with CL, resulting in the smoothest surface morphology and delivering the most effective plasticizing effect. The CL-GLY film showed a dramatic improvement in flexibility, with an elongation at break that was 5.2 times higher than that of the unplasticized film (increasing from 5.39% to 33.14%), indicating significant enhancement in extensibility. Overall, these findings highlight the potential of CL-GLY films as sustainable and effective materials for food packaging applications.

The good oxygen barrier and hydrophobic properties of curdlan (CL) film might be suitable complements for MC film, and its similar glucose unit and thermal-gel character might endow the methyl cellulose (MC)/CL blended system with compatibility and good comprehensive properties. Thus, MC/CL blended films were developed. The effects of MC/CL blend ratios on the microstructures and physical properties of the blends were characterized by using Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), scanning electron microscopy (SEM), oxygen and water vapor permeability testing, dynamic mechanical analysis (DMA), light transmittance testing, tensile testing, hydrophilic property testing, and water solubility testing. The introduction of CL affected the molecular aggregation and crystallization of the MC molecules, suggesting MC–CL molecular interactions. The cross-sectional roughness of the MC/CL film increased with an increase in CL content, while the surface of the MC/CL 5:5 film was smoother than those of the MC/CL 7:3 and 3:7 films. Only one glass transition temperature, which was between that of the MC and CL films, was observed for the MC/CL 7:3 and MC/CL 5:5 films, indicating the good compatibility of the MC and CL molecules at these two blend ratios. The hydrophobicity and water insolubility increased with the CL content, which was due to the combined effects of more hydrophobic cavities in the CL triple-helix and increased surface roughness. Increased oxygen barrier properties with increasing CL content might be a combined effect of the increased hydrogen bonds and hydrophilic ektexines of the CL triple-helix. The elongations of the blended films were higher than those of the MC film, which might be related to its increased water content. The MC/CL 7:3 and MC/CL 5:5 films retained the good light transmittance and tensile strength of the MC film, which corresponded well to their good compatibility and might be due to the effects of the MC–CL molecular interactions and the relative smooth morphologies. MC/CL 5:5 showed improved water vapor barrier properties, which might be due to its smooth surface morphologies. This research offers new MC based films with improved properties and good compatibility, providing great potential for use as edible coatings, capsules, and packaging materials.