The benzodiazepines, namely 1, 5-Diacetyl-2, 2, 4-trimethyl-1H-tetrahydro-1, 5-benzodiazepine (C16H22N2O2), (DARTMBD, CCDC 716181) and N-5-Ethoxycarbonyl-2-methyl-2, 4-diphenyl-1H-tetrahydro-1, 5-benzodiazepine (C25H26N2O2), (ECRPMBD, CCDC 716182) possess potential pharmacological activities. DARTMBD crystallizes in monoclinic space group P2(1)/c with cell parameters: a = 10.0582(3) angstrom, b = 9.6019(3)degrees, c = 16.0837(4)degrees, beta = 103.100(1)degrees, and V = 1512.91(8)degrees(3); ECRPMBD crystallizes in triclinic system, P (iota) over bar with two crystallographically independent molecules in the asymmetric unit. The cell parameters are: a = 12.2807(4)degrees, b = 12.8410(5)degrees, c = 13.9714(4)degrees, alpha = 90.626(2)degrees, beta = 105.200(3)degrees, gamma = 100.324(2)degrees, and V = 2087.84(12)degrees(3). Both the structures were solved by direct methods and refined by full-matrix least-squares procedures to final R-values of 0.0552 and 0.0487, respectively. The benzodiazepine ring in both the structures adopts twist-boat conformation. In DARTMBD, the dimer formation occurs through C-H center dot center dot center dot O intermolecular interactions whereas in ECRPMBD, the molecules are stabilized by N-H center dot center dot center dot O, and C-H center dot center dot center dot O types of hydrogen bonds.