Abstract By crystal engineering of molecular magnets, unique magnetic functionalities can be intentionally designed. In this work, we synthesized a novel two-dimensional cyanido-bridged coordination network, [NiII(pz)4]{[NiII(pz)3][WV(CN)8]}2·3.5H2O (NiW, pz = pyrazole), which exhibits metamagnetic behavior. NiW has wavy coordination layers created by two differently sized molecular square ladders and exhibits strong intralayer ferromagnetic interactions. Nevertheless, due to the relatively short interlayer distance, NiW shows spontaneous antiferromagnetic ordering below a Néel temperature of 21 K. By applying an external magnetic field, such antiferromagnet can be converted into a ferromagnet with a coercive field of 600 Oe at 2 K, elucidating the metamagnetic behavior of NiW.

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