The progress of unconventional superconductors at the two-dimensional (2D) limit has inspired much interest. Recently, a new superconducting system was discovered in the semimetallic ternary Bi–O–S family. However, pure-phase crystals are difficult to synthesize because of the complicated stacking sequence of multiple charged layers and similar formation kinetics among ternary polytypes, leaving several fundamental issues regarding the structure–superconductivity correlation unresolved. Herein, 2D single-crystal ultrathin Bi3O2S3 nanosheets are prepared by using low-pressure chemical vapor deposition, and their atomic arrangement is clarified. Magnetotransport measurements indicate a superconducting transition at ∼6.1 K that is thickness-independent. The transport results demonstrate 2D superconducting characteristics, such as the Berezinskii–Kosterlitz–Thouless transition, and strong anisotropy with magnetic field orientations following the 2D Tinkham formula. The difference from superconductivity of powder is demonstrated from the perspective of their corresponding microstructures. These results corroborate the superconducting behavior of Bi3O2S3, providing fresh insights into the search for other bismuth oxychalcogenides and derivative BiS2-based analogues at the 2D limit.