This contribution reports the preparation of a composite material based on a natural zeolite rich in calcium, stilbite, on which surface nanosized hydroxyapatite is grown under controlled conditions. Low crystallisation temperatures enable the crystallisation of nano-sized hydroxyapatite crystals, which display a very high intrinsic capacity (based on weight of hydroxyapatite) of fluoride removal. The low cost and easy accessibility of the materials employed for its preparation, as well as the simplicity of the synthesis procedure, make these materials suitable candidates for their use in fluoride removal from drinking water.