Single‐unit‐cell orthorhombic CoSe2 sheets are prepared by thermally exfoliating a lamellar CoSe2–DETA hybrid. As shown by Y. Sun, S. Wei, Y. Xie et al. in their Communication on page 12004 ff., the single‐unit‐cell thickness means that 66.7 % of the Co2+ ions are exposed on the surface and are low coordinate (coordination numbers of 1.3 and 2.6), leading to a lower Tafel slope (64 mV dec−1) and a higher turnover frequency (745 h−1) in water splitting.