In this article, we report a clean and time-effective solvothermal synthesis route using microwave-assisted heating method to prepare nanocrystalline anatase TiO2 with its application for dye-sensitized solar cells. With this proposed method, pure anatase TiO2 nanoparticles with size about 20 nm are successfully obtained at 220 °C for 30 min. Our method of microwave-assisted organic solvothermal route significantly reduces the elaborating process of washing and solvent exchange for the subsequent paste formation. The as-synthesized TiO2 colloidal solution is ready for particle dispersion that markedly simplified the preparation procedures. Material characterizations of the anatase TiO2 nanoparticles are performed by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS), respectively. The photovoltaic performances of the dye-sensitized solar cells assembled with the as-synthesized TiO2 nanocrystallines as photoanodes in various film thicknesses are examined. An excellent energy conversion efficiency of 7.8% is achieved which is comparable to the previously reported dye-sensitized solar cells made of hydrothermal microwave-synthesized TiO2.