Polysaccharides are abundant in nature, renewable, nontoxic, and intrinsically biodegradable. They possess a high level of functional groups including hydroxyl, amino, and carboxylic acid groups. These functional groups can be utilized for further modification of polysaccharides with small molecules, polymers, and crosslinkers; the modified polysaccharides have been used as effective building blocks in fabricating novel biomaterials for various biomedical applications such as drug delivery carriers, cell-encapsulating biomaterials, and tissue engineering scaffolds. This review describes recent strategies to modify polysaccharides for the development of polysaccharide-based biomaterials; typically self-assembled micelles, crosslinked microgels/nanogels, three-dimensional hydrogels, and fibrous meshes. In addition, the outlook is briefly discussed on the important aspects for the current and future development of polysaccharide-based biomaterials, particularly tumor-targeting intracellular drug delivery nanocarriers.

Biopolymer-based nanogels (bionanogels) are a promising platform as polymer-based drug delivery systems encapsulting hydrophilic anticancer therapeutics; however, enhanced/controlled drug release is highly desired. Herein, we report new dual stimuli-responsive bionanogels (ssBNGs) as potential intracellular delivery nanocarriers with multi-controlled and enhanced drug release. A facile aqueous crosslinking polymerization of oligo(ethylene oxide)-containing methacrylate (OEOMA) in the presence of carboxymethyl cellulose (CMC) and a disulfide-labeled dimethacrylate allows for the synthesis of ssBNGs crosslinked with disulfide linkages of POEOMA-grafted CMC. These ssBNGs exhibit dual response release of encapsulated anticancer drugs: reductive cleavage of disulfide crosslinks and acidic pH-response of carboxylic acid groups in CMC. Their applicability toward tumor-targeting drug delivery applications is demonstrated with confocal laser scanning microscopy for cellular uptake and cell viability, as well as a facile bioconjugation with a water-soluble UV-active dye as a model cell-targeting biomolecule.

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