Graphical Abstract 2-nm-thick indium oxide nanosheets with high electron mobility have been synthesized utilizing a liquid metal printing technique and thermal annealing in air. Transmission electron microscopy with in situ annealing reveals that the improvement in device performances is due to nanostructural changes during annealing process. This work highlights a facile and ambient air compatible method for fabricating high-quality semiconductors, which find application in emerging electronics and optoelectronics.