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Aminoglycosides are a family of naturally isolated or chemically semi‐synthesized antibiotics consisting of aminocyclitols with several amino and saccharide units. The unique molecule structures render aminoglycosides promising building blocks with high reactivity to perform various non‐covalent and covalent reactions, and they are further employed to rationally fabricate versatile materials, such as hydrogels, amphiphiles, hyperbranched polymers, biointerfaces, and nanoparticles. Despite aminoglycosides are widely used in clinics to treat bacterial infections, almost all the efforts are focused on molecular modifications to reduce their toxicities and overcome antibiotic resistance, while their actions as building blocks to construct biomaterials are scarcely discussed. In this feature article, the current progress on the rational design, emergent properties, and promising biological applications of aminoglycoside‐based biomaterials are summarized. It is believed that this paper may provide guidance to develop new biomaterials using natural functional molecules as building blocks, and start a new life of aminoglycosides from the view of materials science.

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All-small-molecule smart hydrogels fabricated by naturally occurring and commercially available small molecular building blocks have attracted increasing interest due to their unique features such as biofunction integration and multi-stimuli responsiveness. While a few examples have been well-explored, the further development of additional kinds of all-small-molecule smart hydrogels is severely hindered by the lack of enough commensurate building blocks from nature and market. Therefore, it is crucial to seek new strategies to expand the scope of all-smallmolecule dynamic covalent hydrogels using well-established natural and commercial chemicals. Herein, this issue is addressed by introducing a bifunctional adapter bearing an aldehyde group and a boronic acid group to construct a novel all-small-molecule smart hydrogel through the dynamical covalent cross-linking with naturally occurring building blocks (e.g., tobramycin and tannic acid). The prepared hydrogel presents several promising features including tunable mechanical property, multi-stimuli responsiveness, controlled drug release profiles, and excellent in vitro and in vivo antibacterial performances. This study provides a new strategy to efficiently expand the scope of the all-small-molecule smart hydrogels via the integration of the naturally occurring building blocks and the bifunctional adapters.

Antibiotic hydrogels with sustained release profiles are recognized as promising candidates to treat local bacterial infections with reduced adverse effects. However, it still remains challenging for clinical translation of these antibiotic gels due to safety concern of gel ingredients, complicated synthesis and fabrication procedures, and unsatisfactory rheological properties for practical uses in vivo. Herein, the preparation of a type of sprayable hydrogels by ionic interactions between aminoglycosides and cellulose nanocrystals (CNC) is proposed for the treatment of local infections such as bacteria-infected wounds. The CNC-based hydrogels are applicable for all kinds of aminoglycoside antibiotics and show excellent gel stability and rheological behaviors such as shear thinning and fast self-healing, allowing facile administration by injection or spraying. The hydrogels exhibit efficient antibacterial activity both in vitro and in vivo, and accelerate bacteria-infected wounds by spraying on the infected area. The proposed hydrogels by simply mixing of aminoglycosides and CNC provide great prospects for clinical translation in the treatment of local infections.