The six-fold symmetry possessed by the (111) surfaces of perovskite oxides allows the epitaxial growth of novel quantum materials such as topological insulators. The dielectric SrTiO3(111) thin film is an ideal buffer layer, providing the readily tunability of charge density in gate-controlled structures. But the high-quality film growth is challenging due to its strong surface polarity as well as the difficulty of obtaining the chemical stoichiometry. Here we show that the layer-by-layer growth of homoepitaxial SrTiO3(111) thin films can be achieved in molecular beam epitaxy method by keeping the growing surface reconstructed. And the cation stoichiometry is optimized precisely with the reflective high energy electron diffraction as the feedback signal that changes sensitively to the variation of metal concentration during growth. With atomically well-defined surfaces, the SrTiO3(111) films show high dielectric performance with the charge density modulated in the range of 2 × 10(13)/cm(2) with the back gate voltage lower than 0.2 V. Methods of further broadening the range are also discussed.