The invention discloses a preparation method of a silicon dioxide/nickel core-shell nano-structure material. The preparation method comprises the following steps: preparing SiO2 microspheres, dispersing the SiO2 microspheres in water, mixing the SiO2 microspheres with cationic polyelectrolyte to obtain positively charged SiO2 microspheres after modification, dispersing the positively charged SiO2microspheres in water, mixing the positively charged SiO2 microspheres with an anionic polyelectrolyte to obtain negatively charged SiO2 microspheres after modification, mixing the negatively chargedSiO2 microspheres, a soluble salt of nickel, sodium citrate, lactic acid and water, uniformly stirring the materials, adding a reducing agent into the mixture, and reducing the mixture to obtain the silicon dioxide/nickel core-shell nano-structure material. According to the preparation method, the surface of silicon dioxide does not need an activating treatment process, the process is simple, theperformance is controllable, the production period is short, the production energy consumption is greatly reduced, and the preparation method is suitable for large-scale industrial production. In thefinally prepared product, the nickel content and the thickness of the nickel shell are adjustable and the purity of the nickel coating is high.