Morphologically complex amorphous calcium phosphate nanostructures are synthesized within supersaturated water-in-oil miniemulsions stabilized by a mixture of a calcium bis(2-ethylhexyl)phosphate (Ca(DEHP)2) surfactant and poly(ethylene oxide)19-poly(propylene oxide)69-poly(ethylene oxide)19 (P123) triblock copolymer. Solvent evaporation at room temperature results in self-supporting viscous organogels comprising an interconnected network of calcium phosphate nanofilaments embedded within a continuous polymer/surfactant matrix. The P123/DEHP/calcium phosphate organogels are employed as a bioactive filler for the occlusion of exposed dentine tubules using a standard bovine tooth model.