Fifteen new hydrogen-bonded crystals exhibiting nonlinear optical properties were obtained. For the morpholinium dihydrogenphosphate crystal, the structure was determined by the X-ray diffraction methods. This crystal belongs to the P21 space group of the monoclinic system. The lattice parameters are as follows: a=8.345(2), b=6.156(1), c=9.109(2)Å; β=116.64(3)°. The crystal is built up of the layers parallel to the (001) crystallographic planes. The layer consists of the dihydrogenphosphate chains running parallel to the [010] direction. The morpholinium cation participates in two hydrogen bonds with the O(4) oxygen atoms of dihydrogenphosphate anions belonging to two neighbour chains shifted by the a distance. In such a way, the chains of dihydrogenphosphates are joined by the morpholinium cations into the layer parallel to the (001) crystallographic plane. Additionally, the powder IR and Raman spectra are presented for this crystal.