Neutron scattering studies on low-dimensional quantum spin systems require large-size single-crystals. Single-crystals of (CH3)(2)NH2CuCl3 showing low-dimensional magnetic behaviors were grown by a slow solvent evaporation method in a two-solvent system at different temperature settings. The best results were obtained for the bilayer solution of methanol and isopropanol with a molar ratio of 2:1 at 35 degrees C. The quality of the obtained single-crystals was tested by powder and single-crystal X-ray diffraction and single-crystal neutron diffraction. In addition, to confirm structural phase transitions (SPTs), thermal analysis and single-crystal X-ray diffraction at 300 K and 175 K, respectively, were conducted, confirming the presence of a SPT at T-up= 88 K on heating and T-down=285 K on cooling. (C) 2016 Elsevier B.V. All rights reserved.