Abstract Spintronics applications in two-dimensional (2D) magnetic materials can significantly contribute to the miniaturization and energy efficiency of semiconductor devices. However, current 2D ferromagnetic materials face challenges such as ferromagnetic instability and low Curie temperature (Tc), which limit their broader application. In this study, 2D room-temperature ferromagnetic LaAlO3 was successfully prepared with supercritical carbon dioxide (SC CO2). With the enhanced stress effect of CO2 molecules, the contents of oxygen vacancies OV, aluminium vacancies AlV, and AlO4 in the 2D structure are elevated, and then the ferromagnetic properties of LaAlO3 appeared to be significantly enhanced due to defects and spatial symmetry breaking of the octahedron. Notably, the 2D intrinsic ferromagnetic LaAlO3 exhibited a Tc above 350 K. Therefore, this work supplies a new means for SC CO2 to modulate the microstructure and ferromagnetic properties of 2D LaAlO3, which is conducive to expanding the applications of LaAlO3.