The invention belongs to the field of biomimetic synthetic inorganic materials, and particularly relates to a method for preparation of shape-controllable spinous spherical barium sulfate particulates by taking hydrogen peroxide water solution as a structure regulator. The method includes: adding an inorganic alkali water solution into a hydrogen peroxide water solution with a mass concentration of 0.2-2% to adjust the pH value of the hydrogen peroxide water solution to 11-13.5, and injecting a sulfate water solution and a barium salt water solution or a barium hydroxide water solution with a same mole concentration into the hydrogen peroxide water solution, thus obtaining a mixed solution; when obvious turbidity is generated in the mixed solution, stopping injecting the sulfate water solution and the barium salt water solution or the barium hydroxide water solution, carrying out static ageing at room temperature; and conducting separation and drying, thus obtaining the spinous spherical barium sulfate particulates. The method provided in the invention has the characteristics of wide material sources, energy saving, simple operation, no discharge of three wastes, and the prepared spinous spherical barium sulfate particulates have controllable shapes, so that the method has the potential of mass production. The spinous spherical barium sulfate particulates are expected to have wide application in reinforcing and toughening of materials.