Two new hydrazone compounds, 4-formylimidazole-4-hydroxybenzhydrazone dihydrate (1) and 2-nitrobenzaldehyde-2-furan formylhydrazone (2), were synthesized via the classical synthesis method. Their structure was determined via elemental analysis and X-ray single crystal diffraction analysis. Compound 1 crystallizes in triclinic, space group P-1 with a = 7.0321(14) angstrom, b = 7.3723(15) angstrom, c 13.008(3) angstrom, alpha = 98.66(3)degrees, beta = 101.69(3)degrees, gamma = 92.25(3)degrees, V = 651.2(2) angstrom(3), Z = 2, Dc = 1.358 g.cm(-3), mu = 0.106 mm(-1), F(000) = 280, and final R1 = 0.0564, wR(2) = 0.1420. Compound 2 crystallizes in monoclinic, space group P2(1)/c with a = 17.3618(9) angstrom, b = 9.1506(4) angstrom, c 15.5801(7) angstrom, beta = 104.532(5)degrees, V 2396.05(19) angstrom(3), Z = 8, Dc = 1.437 g.cm(-3), mu = 0.111 mm(-1), F(000) = 1072, and final R-1 = 0.0633, wR(2) = 0.1649. Compound 1 forms a 2D-layered structure via the interactions of 1D chains and Compound 2 forms a 3D network structure via the interactions of 1D chains.