The invention discloses a 3D graphene modified zirconium hydroxide compound adsorbing material for removing fluorinion from rural drinking water and a preparation method thereof. The preparation method comprises the following steps: (1) preparing graphene oxide; (2) preparing a 3D graphene gel; (3) soaking the 3D graphene gel in a mixed solution of a zirconium oxychloride solution and a urea solution and heating in water bath, thereby acquiring the 3D graphene modified zirconium hydroxide compound adsorbing material. According to the invention, the preparation technology is simple; the source of raw materials is wide; the cost is low; the prepared 3D graphene modified zirconium hydroxide compound adsorbing material is high in adsorption capacity for fluorinion and is high in defluorination efficiency; when the prepared 3D graphene modified zirconium hydroxide compound adsorbing material is used for removing the water sample in fluorinion concentration of 25-100mg/L under room temperature, the removing efficiency can reach up to 85% or above.