The preparation, X-ray crystal structure, fourier transform infrared (FTIR) spectroscopy, and elemental analysis of three compounds based on diethylenetriamine and aromatic carboxylic acids are reported. XRD and FTIR analysis indicated that all these complexes are organic salt. The compound 1 crystallizes in the triclinic, space group P-1, with a = 8.5665 (8) Å , b = 11.8387(9) Å , c = 12.4901(11) Å , a = 77.2580(10)°, b = 77.1820(10)°, c = 78.290(2)°, V = 1,188.81(18) Å 3 , Z = 2. The compound 2 crystallizes in the triclinic, space group P-1, with a = 8.0040(7) Å , b = 9.4869(8) Å , c = 20.3491(18) Å , a = 84.6370(10)°, b = 87.032(2)°, c = 78.9620(10)°, V = 1,509.0(2) Å 3 , Z = 2. The compound 3 crystallizes in the orthorhombic, space group Pbca, with a = 12.1232(11) Å , b = 13.5714(14) Å , c = 26.179(3) Å , a = 90°, b = 90°, c = 90°, V = 4,307.3(7) Å 3 , Z = 8. The supramolecular architectures of 1-3 involve extensive hydrogen bonding including N-HÁÁÁO, N-HÁÁÁN, and O-HÁÁÁO interactions as well as other non-covalent CH-O, CH 2 -O, O-p, NH 3? -p, CH 2 -p, and pÁÁÁp interactions, giving 3D framework structures.