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In the present study, polysaccharide-based cryogels demonstrate their potential to mimic a synthetic extracellular matrix. Alginate-based cryogel composites with different gum arabic ratios were synthesized by an external ionic cross-linking protocol, and the interaction between the anionic polysaccharides was investigated. The structural features provided by FT-IR, Raman, and MAS NMR spectra analysis indicated that a chelation mechanism is the main process linking the two biopolymers. In addition, SEM investigations revealed a porous, interconnected, and well-defined structure suitable as a scaffold in tissue engineering. The in vitro tests confirmed the bioactive character of the cryogels through the development of the apatite layer on the surface of the samples after immersion in simulated body fluid, identifying the formation of a stable phase of calcium phosphate and a small amount of calcium oxalate. Cytotoxicity tests performed on fibroblast cells demonstrated the non-toxic effect of alginate–gum arabic cryogel composites. In addition, an increase in flexibility was noted for samples with a high gum arabic content, which determines an appropriate environment to promote tissue regeneration. The newly obtained biomaterials that exhibit all these properties can be successfully involved in the regeneration of soft tissues, wound management, or controlled drug release systems.

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