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The preparation of hollow silica spheres via the sodium silicate route presents many advantages such as a low-cost silica source, and an environmentally friendly reaction system. Unfortunately, it is extremely hard to prepare the well-defined hollow silica spheres by using sodium silicate as the silica source owing to its rapid, disordered precipitation under the acid catalysis. As a result, we, in this paper, report a facile, economic, one-pot pathway for preparation of the ordered hollow silica spheres by employing a sodium silicate precursor. In this approach, the cationic polystyrene (CPS) templates can be first prepared via emulsifier-free emulsion polymerization by using the cationic monomer vinylbenzyltrimethylammonium chloride, then, the silica shells were attached on the surfaces of CPS particles via electrostatic interaction, finally CPS particles were in situ dissolved and removed by adding toluene to create ordered hollow silica spheres. Some modern techniques and instruments, including the transmission electron microscope, scanning electron microscopy, infrared spectroscopy, thermogravimetric analysis, and Brunauer-Emmett-Teller theory were employed to monitor and characterize the resulting hollow silica spheres. [ABSTRACT FROM AUTHOR]