The socioeconomic demand for biomaterials has never been greater. Formulation at the organic/inorganic interface of materials has enabled the conception of several biomaterial systems for bone healing. In Chapter 2, a poly( ether ether ketone) (PEEK) and calcium sulphate (CS) composite is formulated. Inclusion of the polymer slowed CS degradation and augmented the mechanical properties significantly. Chapters 3 and 4 explore the formation mechanism of tubular calcium phosphate structures from a gel/solution interface. Both the composition and microstructure of tubules were analogous to features of bone. To demonstrate the bone graft application of these structures, a model bone defect was augmented with particles that could generate tubular calcium phosphate in the presence of tissue. 3D computed tomography reconstructions revealed bone-like mineral deposition throughout the cavity. Chapter 5 explores the chemical coupling of hydroxyapatite particles within a PEEK matrix, a composite that may be used to fabricate spinal fusion devices. Physical properties of composites were improved by a reduction in HA debonding, the presence of fewer micro cracks, and more effective load transfer between phases. Together, the research puts forward a novel collection ofbiomaterials that may be applied to the treatment of bone fractures and fusion of the spine.