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Based on a strategy of incorporating the SCN − group into the organically templated halocadmate, the reactions of CdCl 2 , SCN − , and bisimidazole molecules in a strong acidic environment at 4 °C were carried out, creating two new organically templated 2-D layered thiocyanato-chlorocadmates [H 2 (L1)][Cd 2 Cl 5 (SCN)] (L1 = bis(1H-imidazole-1-yl)methane) 1 and [H 2 L2] 2 [Cd 5 Cl 12 (SCN) 2 ] (L2 = 1,3-bis(2-ethylimidazol-1-yl)propane) 2 . Both layers are based on a kind of tetranuclear Cd–Cl cluster. Since the employed organic cations are different, the neighboring tetranuclear Cd–Cl clusters are linked together by the different bridges into the 1-D endless chains. In 1 , the Cl − ions act as the bridges, while in 2 , the CdCl 6 units serve as the bridges. Finally, the 1-D Cd–Cl chains are further linked by SCN − into the 2-D layer networks of 1 and 2 . Both layers possess a simple (4,4) topology. Based on the structural characterization of the title compounds, the role of the introduced SCN − group on the organically templated halocadmates is discussed. [ABSTRACT FROM AUTHOR]