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Copper(II) silver(II) sulfate crystallizes in a monoclinic CuSO 4 ‐related structure with  P 2 1 / n  symmetry. This quasi‐ternary compound features Ag(SO 4 ) 2  2−  layers, while the remaining cationic sites may be occupied either completely or partially by Cu 2+  cations, corresponding to the formula of (Cu  x  Ag 1− x  )[Ag(SO 4 ) 2 ],  x =0.6−1.0. CuAg(SO 4 ) 2  is antiferromagnetic with large negative Curie‐Weiss temperature of −140 K and shows characteristic ordering phenomenon at 40.4 K. Density functional theory calculations reveal that the strongest superexchange interaction is a two‐dimensional antiferromagnetic coupling within Ag(SO 4 ) 2  2−  layers, with the superexchange constant  J  2D  of −11.1 meV. This renders CuAg(SO 4 ) 2  the rare representative of layered Ag 2+ ‐based antiferromagnets. Magnetic coupling is facilitated by the strong mixing of Ag  d ( x  2 − y  2 ) and O 2 p  states. Calculations show that M 2+  sites in MAg(SO 4 ) 2  can be occupied with other similar cations such as Zn 2+ , Cd 2+ , Ni 2+ , Co 2+ , and Mg 2+ .

A Unique Two‐Dimensional Silver(II) Antiferromagnet Cu[Ag(SO 4 ) 2 ] and Perspectives for Its Further Modifications