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SnO2 solid microspheres and multilayered nanocrystalline SnO2 hollow microspheres (MHS-SnO2) have been successfully synthesized in the solvothermal environment by using different solvents. The morphology, structure and composition of the as-prepared products are characterized by field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), high resolution transmission electron microscopy (HRTEM) with selected area electron diffraction (SAED) and X-ray diffraction (XRD). The growth mechanism of SnO2 solid microspheres and MHS-SnO2 are proposed and attributed to the viscosity of solvent. The studies on hydrogen absorption characteristics of SnO2 solid structure and MHS-SnO2 show an absorption capability of 0.50 wt.% and 0.92 wt.%, respectively.