Mn2(OH)2SO4, obtained as pink prismatic crystals by the hydrothermal reaction of MnSO4·H2O and NaOH at 240 °C for 24 h, consists of layers of Mn hydroxide connected to each other through µ6‐sulfate ions. Each layer exhibits vacancies, and each vacant space is capped at the top and bottom by the sulfate groups. The compound is paramagnetic above 50 K (C = 4.36 emu K mol−1, µeff = 5.91 µB, Θ = −100 K). Below 45 K, the magnetization increases slightly, indicating canted‐antiferromagnetic (TNéel = 42±1 K) behavior consistent with the linear dependence of the magnetization as a function of the field at 2 K, which reaches only 0.4 µB at 50 kOe, and the lack of any imaginary component of the ac‐susceptibilities (ac = alternating current). (© Wiley‐VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2004)