Hemicellulose and polyphenols present attractive functional potential for the elaboration of biobased materials but their interaction remains scarcely studied. In this study, the interaction behavior of xyloglucan (XG) and tannic acid (TA) was systematically studied over XG concentration ranging from 0.25g/L to 3g/L and TA:XG weight ratio from 0.1 to 10. Three distinct types of assemblies identified as swollen coils, dense beads or aggregated beads were described using a combination of QCM-D, light scattering and thermodynamic characterizations. They differed in size and colloidal behavior, and their formation was primarily governed by hydrophobic interactions and steric repulsions. These findings provide new insights into the molecular mechanisms driving hemicellulose-polyphenol association and highlight their potential in the design of functional, plant-inspired materials.

Engineering bioinks that integrate printability, mechanical stability, and osteoconductivity remains a significant challenge for generating mineralizing bone tissue models. While numerous gelatin methacrylate (GelMA)-based bioinks have been developed, comprehensive demonstration of cell-mediated, apatite-like mineral formation within bioprinted constructs remains limited. Here, we present a synergistic gelatin-methacrylate/κ-carrageenan (GelMA/κCGN) composite hydrogel that couples printability with mineralization potential. Incorporation of κCGN increases pre-gel viscoelasticity, improves shear-thinning, and maintains rapid photocrosslinking of GelMA, enabling uniform filament extrusion, multilayer stacking, and high shape fidelity. The composite hydrogels display reinforced compressive properties and improved structural stability compared to GelMA. Human mesenchymal stem cells (hMSCs) embedded in these constructs remain viable and exhibit a strong osteogenic programme. Histological staining demonstrates abundant collagen matrix deposition, accompanied by calcium accumulation. Localized SEM-EDS compositional analysis of discrete domains reveals calcium‑phosphorus co-localization and Ca/P ratios consistent with early-stage, calcium-deficient apatite-like phases, supporting cell-mediated matrix mineralization within the 3D hydrogel microenvironment. Bioprinted constructs retain these characteristics, supporting homogeneous cell distribution, sustained osteogenic differentiation, and robust matrix deposition. Collectively, these findings demonstrate that engineered GelMA/κCGN composite hydrogels, integrating optimized rheological performance with biologically driven, apatite-like mineralization, offer a promising platform for bone tissue engineering and advanced in vitro models.

Biobased materials are increasingly being developed to replace petroleum-derived counterparts as renewable, recyclable, biodegradable, and environmentally friendly packaging products. This review focuses on starch-based biopolymers, given their abundance in the global supply chain and their potential to produce high-barrier, mechanically robust composites, films, and coatings. The barrier and mechanical performance of starch-based materials is critically examined, with emphasis on structure-property relationships. Key physical and chemical modification strategies used to overcome the inherent limitations of native starch are discussed, with a particular focus on citric acid crosslinking as a scalable and environmentally friendly approach for enhancing barrier performance in commercial packaging applications. Crosslinking starch with citric acid, a naturally derived multifunctional carboxylic acid, significantly improves the physical, chemical, morphological, thermal, crystalline, and hydrophobic properties of starch films and coatings. Optimal performance is achieved through precise control of processing parameters, including pH, temperature, citric acid concentration, plasticizer levels, and curing conditions. Importantly, citric acid crosslinking imparts enhanced structural stability while preserving the recyclability, compostability, and biodegradability of starch-based materials, consistent with green chemistry principles. Overall, this review highlights citric acid-crosslinked starch as a promising platform for circular packaging solutions aligned with Extended Producer Responsibility (EPR) frameworks and European Union (EU) regulatory requirements.