The two novel (R/S-ClMBA)2CuCl4 chiral compounds crystallize in the noncentrosymmetric C2 space group in analogy with (R/S-MBA)2CuCl4. Note that the crystallographic data reported for the last two samples are herein collected under the same conditions (i.e., wavelengths and temperature) as the present novel ClMBAcontaining compounds and have therefore redeposited in the database for consistency. Figure reports a sketch of the crystal structure for (R/S-ClMBA)2CuCl4 along different projections, while a picture of the aspect of the green crystals is reported in Figure . The analogous plots for (R/S-ClMBA)2CuCl4 are shown in the Supporting Information (Figure ). The structural arrangement of (R/S-ClMBA)2CuCl4 resembles that of the MBA analogue, with a lamellar structure of isolated CuCl4 tetrahedra and a bilayer of organic ligands. The Cl of the benzene ring points inside such bilayer while the protonated amino group is directed towards the chloride of the tetrahedron. There is a clear expansion of )