The invention discloses a three-dimension carbon cloth/nickel iron layer shaped hydroxide nanosheet composite material and application thereof. A preparation method of the material comprises the following steps: putting carbon cloth into 3 mol/L nitric acid, and enabling the components to react for 2 hours at a reaction temperature of 120 DEG C so as to obtain functionalized three-dimensional carbon cloth; soaking the functionalized three-dimensional carbon cloth into a mixture of ferric nitrate, nickel nitrate, urea and ammonium fluoride, enabling the components to react for 6-10 hours at a reaction temperature of 100-120 DEG C, cooling to a room temperature, washing, and drying, thereby obtaining the three-dimension carbon cloth/nickel iron layer shaped hydroxide nanosheet composite material. The three-dimension carbon cloth/nickel iron layer shaped hydroxide nanosheet composite material can be connected with a working electrode for detecting nitrate ions in water. The material is simple in preparation method, high in charge transfer efficiency, capable of rapidly, efficiently and selectively detecting nitrate ions in the water body relatively wide in linear detection range and relatively low in detection limit.