The conventional V2O5 preparation processes include ion exchange, chemical precipitation, solvent extraction, and other processes. Given the long process and complex operation nature of traditional V2O5 production methods, we herein developed a short-process, low-temperature, and convenient operation method of isolating vanadium (in the form of V2O5) from shale acid leaching solution. The acid leaching solution was oxidized with NaClO3 and pH-adjusted with NaOH to form a vanadium-containing precipitate, which was mixed with AlCl3 (V:AlCl3 = 1:5, mol/mol) and roasted for 120 min at 170 °C to afford vanadium oxytrichloride (VOCl3) with a purity of 99.59%. In addition, the vanadium-containing precipitate was mixed with AlCl3 and NaCl (V:AlCl3:NaCl = 3:12:8, mol/mol/mol) and roasted for 120 min at 170 °C to afford VOCl3 with a purity of 99.94%. VOCl3 (purity of 99.94%) was dissolved in ultrapure water, and the solution (32 gvanadium/L) was treated with NH3·H2O (NH3:V = 1.34, mol/mol) at 50 °C for 120 min. The obtained precipitate (vanadium precipitation rate = 99.28%) was roasted at 550 °C for 3 h to afford high-purity vanadium pentoxide (V2O5) with a purity of 99.86%. Compared with the traditional hydrometallurgical method of V2O5 preparation, our method avoided solvent extraction and other undesired processes and the overall process flow is greatly shortened, thus having high practical value.