Bovine dentine has been used as a template for the electrochemical crystallization of copper microwires, and as a target surface for two amorphous calcium phosphate (ACP) mediated remineralization vectors. When used as a macroporous template, spatially separated co-aligned arrays of copper microwires were synthesized within the dentine tubules by electrochemical deposition. The high-aspect ratio wires were continuous throughout the dentine matrix, 1-4 11m in thickness and rendered the composite material electrically conductive with enhanced mechanical hardness. A macromolecular-rich, coacervate phase, self assembled from the mixing of aqueous solutions of poly(diallyldimethylammonium) chloride (PDDA) and poly(ethylene glycol) 4-nonylphenyl 3-sulfopropyl ether potassium salt (51) was used as a synthetic medium and delivery vector for ACP nanoparticles to the dentine surface. Physical characterization of the coacervate phase showed dispersions of droplets of differing surface charge, water content and size could be prepared by alteration of initial component stoichiometries. The high concentration of macromolecules present within the coacervate phase enhanced the meta-stability of the amorphous particles and imparted morphological control on the ACP spherules. Preliminary studies to determine viability of the coacervate as a delivery vector for the ACP-mediated occlusion of dentine tubules showed improved mineral penetration and tubule occlusion in comparison with control assays. The remineralization capacity of hybrid, electrospun mats of the polymer poly(vinylpyrrolidone) (PVP) and stabilized (ACP) particles was determined. The ACP particles were characterized by a range of techniques which showed they were amorphous and prone to aggregation. When electrospun from ethanol based solutions with the polymer composite mats comprising amorphous particles 48 % by mass were produced. Assessment of the efficacy of the mats as a vector for the ACP-mediated occlusion of dentine tubules showed the delivery of micrometre scale particles to the dentine surface, which did not form a contiguous surface coverage, or result in tubule occlusion.