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The magnetic properties of a 2D layered material consisting of high-spin Co 2+ complexes, [Co(NH 3 NH 2 ) 2 (H 2 O) 2 Cl 2 ]Cl 2 ( CoHyd 2 Cl 4 ), have been extensively characterized using electron paramagnetic resonance, magnetic susceptibility, and low-temperature heat capacity measurements. Electron paramagnetic resonance spectroscopy studies suggest that below 50 K, the J = 3/2 orbital triplet state of Co is gradually depopulated in favor of the J = 1/2 spin state, which is dominant below 20 K. In light of this, the magnetic susceptibility has been fitted with a two-level model, indicating that the interactions in this material are much weaker than previously thought. This two-level model is unable to fit the data at low temperatures and, combined with electron paramagnetic resonance spectroscopy, suggests that ferromagnetic interactions between Co 2+ cations in the J = 1/2 state become significant approaching 2 K. Heat capacity measurements suggest the emergence of a long-range ordered state below 246 mK, which neutron diffraction confirms to be ferromagnetic., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)