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Antioxidant biomaterials have attracted much attention in various biomedical fields because of their effective inhibition and elimination of reactive oxygen species (ROS) in pathological tissues. However, the difficulty in ensuring biocompatibility, biodegradability and bioavailability of antioxidant materials has limited their further development. Novel bioavailable antioxidant materials that are derived from natural resources are urgently needed. Here, an integrated multi-omics method was applied to fabricate antioxidant biomaterials. A key cysteine-rich thrombospondin-1 type I repeat-like (TSRL) protein was efficiently discovered from among 1262 adhesive components and then used to create a recombinant protein with a yield of 500 mg L−1. The biocompatible TSRL protein was able to self-assemble into either a water-resistant coating through Ca2+-mediated coordination or redox-responsive hydrogels with tunable physical properties. The TSRL-based hydrogels showed stronger 1,1-diphenyl-2-picrylhydrazyl (DPPH) radical scavenging rates than glutathione (GSH) and ascorbic acid (Aa) and protected cells against external oxidative stress significantly more effectively. When topically applied to mice skin, TSRL alleviated epidermal hyperplasia and suppressed the degradation of collagen and elastic fibers caused by ultraviolet radiation B (UVB) irradiation, confirming that it enhanced antioxidant activity in vivo. This is the first study to successfully characterize natural antioxidant biomaterials created from marine invertebrate adhesives, and the findings indicate the excellent prospects of these biomaterials for great applications in tissue regeneration and cosmeceuticals.

Osteoporosis is caused by an osteoclast activation mechanism. People suffering from osteoporosis are prone to bone defects. Increasing evidence indicates that scavenging reactive oxygen species (ROS) can inhibit receptor activator of nuclear factor κB ligand (RANKL)-induced osteoclastogenesis and suppress ovariectomy-induced osteoporosis. It is critical to develop biomaterials with antioxidant properties to modulate osteoclast activity for treating osteoporotic bone defects. Previous studies have shown that manganese (Mn) can improve bone regeneration, and Mn supplementation may treat osteoporosis. However, the effect of Mn on osteoclasts and the role of Mn in osteoporotic bone defects remain unclear. In present research, a model bioceramic, Mn-contained β-tricalcium phosphate (Mn-TCP) was prepared by introducing Mn into β-TCP. The introduction of Mn into β-TCP significantly improved the scavenging of oxygen radicals and nitrogen radicals, demonstrating that Mn-TCP bioceramics might have antioxidant properties. The in vitro and in vivo findings revealed that Mn2+ ions released from Mn-TCP bioceramics could distinctly inhibit the formation and function of osteoclasts, promote the differentiation of osteoblasts, and accelerate bone regeneration under osteoporotic conditions in vivo. Mechanistically, Mn-TCP bioceramics inhibited osteoclastogenesis and promoted the regeneration of osteoporotic bone defects by scavenging ROS via Nrf2 activation. These results suggest that Mn-containing bioceramics with osteoconductivity, ROS scavenging and bone resorption inhibition abilities may be an ideal biomaterial for the treatment of osteoporotic bone defect.