A method for preparing an ultrathin two-dimensional (2D) monocrystalline nanosheet, the method including: 1) placing BiX3 powder where X=I, Br, or Cl in a crucible, and putting the crucible on a first heating zone of a furnace disposed at a gas inlet of a quartz tube; placing substrates covered with metal sheets on a second heating zone of the furnace disposed at a gas outlet of the quartz tube; 2) vacuumizing the quartz tube; pumping Ar gas into the quartz tube until the air pressure is 101.325 kPa; pumping a carrier gas into the quartz tube; and 3) heating and maintaining the second heating zone; heating the first heating zone for BiX3 evaporation until producing chemical reaction between BiX3 and the metal sheets, and preparing ultrathin 2D nanosheets on the substrates simultaneously; and cooling the substrate naturally to 15-30° C.