Cs 3 (HSO 4 ) 2 (H 2 PO 4 ) single crystals, obtained for the first time based on a systematic study of the phase diagram of the CsH 2 PO 4 -CsHSO 4 -H 2 O ternary system, have been studied by X-ray diffraction. The atomic structure of the crystals at room temperature is determined, and their structural features are analyzed.