Controlling the synthesis of atomic-thick nanosheets of nonlayered materials is extremely challenging because of the lack of an intrinsic driving force for anisotropic growth of two-dimensional (2D) structures. In that case, control of the anisotropy such as oriented attachment of small building blocks during the reaction process will be an effective way to achieve 2D nanosheets. Those atomic thick nanosheets possess novel electronic structures and physical properties compared with the corresponding bulk samples. Here we report Co9Se8 single-crystalline nanosheets with atomic thickness and unique lamellar stacking formed by 2D oriented attachment. The atomic-thick Co9Se8 nanosheets were found to exhibit intrinsic half-metallic ferromagnetism, as supported by both our experimental measurements and theoretical calculations. This work will not only open a new door in the search for new half-metallic ferromagnetic systems but also pave a practical way to design ultrathin, transparent, and flexible paperlike spintronic devices.