Materials that enhance bone and cartilage regeneration promise to be valuable in both research and clinical applications. Both natural and synthetic polymers can be used to create scaffolds that support cells and incorporate cues which guide tissue repair. Recently, electrospinning, peptide self-assembly and biomineralisation have been employed to fabricate nanostructured scaffolds that better mimic the complex extracellular environment found within tissues, in vivo. The incorporation of peptide motifs recognised by cell receptors and the use of recombinant DNA technology have enabled the creation of scaffolds with new levels of biofunctionality. Advances in materials design will enhance our ability to create highly tailored cellular environments for bone and cartilage regeneration.