CsNiP and 2(LiZnHP2O7) crystals were synthesized by hydrothermal technique at moderate P-T conditions. Solubility results of both the compound shown positive thermal coefficient and single crystal X-ray studies revealed, CsNiP crystallized in hexagonal system with cell parameters; a = 7.173(2), c = 5.944(9) angstrom, V = 264.87(7) angstrom(3) and space group P63/mmc and 2(LiZnHP2O7) crystallized in orthorhombic system with cell parameters; a = 12.3636 angstrom, b 27.5330 angstrom, c = 6.8647 angstrom and space group, Pca21 exhibiting ring type of cavities with open aperture in the structure. CsNiP is a frequency dependent paramagnetic and 2(LiZnHP2O7) is a diamagnetic. (c) 2006 Springer Science + Business Media, Inc.