Crystals of the organic-inorganic hybrid complex [H3NCH2(C5H4NH)]2CdBr6·2H2O ([H3NCH2(C5H4NH)] = diprotonated 3-picolylamine or 3-ampH2), were grown successfully by slow evaporation solution growth method at room temperature and characterized by single-crystal X-ray diffraction, infrared absorption, optical absorption and thermal analysis. The title compound belongs to the triclinic space group P1 ̅, with a crystal structure consisting of inorganic layers built up from hexabromocadmate anions [CdBr6]4- and free water molecules, linked together by O-H···Br hydrogen bonds and halogen···halogen interactions, along the b axis. The organic cations, 3-ampH2, are intercalated between the mineral layers via N-H···Br hydrogen bonds. The optimized molecular structure and the vibrational spectra were calculated thanks to the Density Functional Theory (DFT) method resorting to the B3LYP function with the LanL2DZ basis set. Infrared spectrum was used to gain more information of the title compound, with the assignment of the observed vibration modes. Good agreement has been found between the calculated results and the experimental data. Subsequently, the optical properties were diagnosed throughout optical absorption explaining the possible charge transfer interactions that happen within the molecules. The thermal behavior was studied by TG/DT analyses. In silico analyses showed that the synthesized compound bound several anticancer receptors (TNF-α, COX-2, VEGF...) with high affinities, which together with molecular interactions, druggability and pharmacokinetics satisfactory explain the anticancer potential of the compound.