In this Article, epitaxial thin films of SrTiO3 were prepared on single crystalline (100) LaAlO3 by an aqueous chemical solution deposition method. By using different chelating agents to stabilize the metal ions in water, the impact of the precursor chemistry on the microstructural and crystalline properties of the films was studied. Thorough investigation of the precursor by means of infrared and Raman spectroscopy as well as thermogravimetric analysis revealed that stable precursors can be obtained in which strontium ions can be either free in the solution or stabilized by one of the chelating agents. This stabilization of strontium ions appeared to be essential in order to obtain single phase SrTiO3 films. Precursors in which Sr2+ remained as free ions showed SrO microcrystal segregation. Precursors in which both metal ions were stabilized gave rise to strongly textured, dense, and terraced SrTiO3 films, allowing subsequent deposition of YBa2Cu3O7-delta with superior superconducting performances.