The invention belongs to the technical field of a soft chemical method. According to the invention, the method is used for overcoming the defects that the traditional solid-phase glass powder method for preparing a hollow glass micro-balloon is high in energy consumption, long in technical process and difficult in controlling grain size distribution and the hollow glass micro-balloon prepared according to a liquid-phase atomizing method is high in alkalinity, easy to absorb water, high in strength and easy to break, and the like. A liquid material system is compounded through a chemical reaction; after the system is homogenized, the system is quickly atomized, dewatered and dried, thereby obtaining approximate spherical precursor powder with required grain size and corresponding distribution; and the powder is treated under high temperature at 600-1100 DEG C, thereby obtaining a micron-scale hollow glass micro-balloon with the volume floating rate being above 90%, the SiO2 content (weight) being 55-88%, the true density being 0.1-0.7g/cm<3> and the compression strength being 1-50MPa. The method is low in energy consumption, free from fusion and sintering, and high in yield. The prepared hollow glass micro-balloon is high in compression strength, light in weight, low-alkali, waterproof, excellent in fluidity and dispersibility, and suitable for various high-performance light compound materials.