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Two-dimensional cesium bimetal cyano-bridgedassemblies CsI4CoII[MoV(CN)8]Cl3(CsCoMo) and CsI4CoII[WV(CN)8]Cl3(CsCoW) were synthesized. The negatively chargedand solvent-free{CoII[MV(CN)8]Cl3}4-(M = Mo, W) coordination layers are separated byCs+ions. Themogravimetric measurements show that thesecompounds reveal high thermal durability up to 523 K (250 °C),which is due to the absence of solvent molecules in their crystalstructures. The magnetic measurements show that CsCoMoand CsCoWare metamagnets showing the field-inducedtransition from an antiferromagnetic phase with Néel temperatureof 25 K to a ferromagnetic phase, which is observed at high criticalmagnetic field of 24 kOe at 1.8 K. These originate from antiferromagneticinteractions between ferromagnetically coupled cyano-bridged CoII-MVlayers, and the contribution from single-ionanisotropy of CoII. [ABSTRACT FROM AUTHOR]