We introduce a single-step lithography process based on Ga+-focused ion beam (FIB) irradiation to trigger a topotactic transformation on SrFeO3−δ thin films, from the perovskite to the brownmillerite (BM) crystal structure. The crystallographic transformation is triggered by preferential oxygen sputtering by Ga+-FIB irradiation, which favors the formation of the SrFeO2.5 BM phase. The transformation has been verified through micro-Raman spectroscopy on thin films subjected to Ga+-FIB irradiation under 5 kV and 30 kV. Inducing crystallographic transformations by FIB in a single-step process (without the need of resists), at a very high speed (low Ga+ doses are required, in the range of 1015 ions/cm2), with very high spatial resolution (limited by the ion beam spot, of a few square nanometers) and with potential for upscaling using broad Ga+ beams, this approach represents a significant forward step over previous methods using multistep lithographic or electrochemical procedures. All these virtues make this process appealing to develop applications based not only on SrFeO3−δ thin films but also on other oxide films harnessing topotactic transformations.