Recent Advances in the Design and Structural/Functional Regulations of Biomolecule-Reinforced Graphene Materials for Bone Tissue Engineering Applications.

Biomolecule-reinforced graphene materials (Bio-RGMs) have emerged as versatile matrices for biomedical and tissue engineering applications, owing to the combination of graphene-based materials (GMs) with biomolecular components and their synergistic effects. In this review, an overview of the design, synthesis, structural/functional regulation, and bone engineering applications of various Bio-RGMs is provided. Both covalent and noncovalent methods for conjugating biomolecules onto GMs, followed by an exploration of the structural diversity of Bio-RGMs, ranging from 1D nanofibers to 2D membranes and 3D scaffolds/hydrogels/aerogels are discussed. Techniques such as electrospinning, self-assembly, freeze-drying, 3D printing, and templated synthesis are highlighted for their roles in designing and fabricating Bio-RGM architectures. Additionally, specific properties and functions endowed to Bio-RGMs by biomolecule conjugation, including biocompatibility, cytotoxicity, antibacterial activity, drug delivery ability, and fluorescent sensing are examined. Finally, recent advance is showcased in fabricating Bio-RGMs for the bone tissue engineering applications of bone repair, regeneration, grafting, drug/cell delivery, and tumor inhibition, and further, the potential of Bio-RGMs for preclinical applications is analyzed. It is believed that this review will deepen readers' understanding of biomolecule-GM interactions and inspire the development of innovative Bio-RGMs for advanced biomedical and tissue engineering applications.