Chemists and physicists have jointly pushed the rapid progress of molecule-based nanomagnets in recent years. [1] Since the first discovery of single-molecule magnets (SMMs) in the 1990s, [2] exciting discoveries in this area have included single-chain magnets (SCMs, or so-called magnetic nanowires) [3] and a hydrogen-bonded SMM dimer, [4] which can be regarded as expansions of SMMs by intermolecular magnetic interactions. [4, 5] These observations have encouraged chemists to construct or tailor SMMs into an extended network with the hope that certain cooperative effects mediated by covalent linkers could improve the quantum properties of the original units. [5][6][7] This idea has led to a variety of interesting SMM networks exhibiting properties from classical to quantum magnetism [6,7] and provided useful subjects for studying the effects of intermolecular interactions on the behavior arising from the energy barrier to magnetization reversal. [4][5][6][7] In contrast to the rapid development of SMM networks, SCM networks are significantly restricted, which may be attributable to the difficulty in arranging these magnetic nanowires while maintaining a sufficiently large ratio of intra-to interchain magnetic interaction to "freeze in" one-dimensional (1D) magnetization and prevent 3D ordering.[3] Thus, it is important to use proper covalent linkers, which should have at least two features: 1) multitopic structure to covalently link the chains; 2) magnetically "inertness" to efficiently prevent magnetic interactions between the chains.As s-bonding linkers are significantly weaker mediators of the spin carriers, [8] crystal engineering with a judicious choice of s-bonding ditopic linkers may allow us to covalently link 1D Ising ferro-or ferrimagnetic chains into 2D or 3D networks without significant deterioration of the one-dimensional magnetism of the SCMs in the 2D or 3D structures, although no genuine example has been reported so far. In this regard, trans-1,2-cyclohexanedicarboxylate (trans-1,2-chdc) is a good candidate, since it was demonstrated to be a very weak magnetic mediator [9] due to alternation effects.[8]As part of our ongoing search for new magnetic coordination polymers, [10] we chose this ligand as a structural linker and magnetic separator to incorporate magnetic anisotropic chains into a higher dimensional network. We have used trans-1,2-chdc to prepare laminated coordination polymer 2 1 [Co II 3 (OH) 2 (trans-1,2-chdc) 2 ] (1) exhibiting magnetism due to coexistent spin frustration and long-range magnetic ordering.[10a] Interestingly, at lower reaction pH value and temperature, we obtained the new laminated product 2 1 [Co II (trans-1,2-chdc)] (2) as a pure phase, which consists of a parallel arrangement of carboxylate-bridged, paddle-wheel Co II chains and shows interesting SCM behavior.In the single-crystal structure of 2, the Co II atom (Figure 1 and Figure S1) adopts a slightly distorted square-pyramidal geometry with four basal oxygen atoms (CoÀO 1.971(3)-2.210(3) ) and one apical oxy...