The dataset is composed of the theoretically optimized structures, energetics and electronic structures information of more than two hundreds of tetrahedral-bonding hybrid heterostructured semiconductors (HHSs). We have given the related information to reproduce the calculations by using the plane-wave pseudopotential methods within the density functional theory with the Perdew-Burke-Ernzerhof exchange-correlation functional as implemented in the Vienna Ab-initio Simulation Package. The file directory is organized as below: |-.Input-files |-.HHSs-CIF |-.Tetrahedral-Bonding HHSs |-.Inorganic_Semiconductors |-.Organic_Molecules |-.HHSs-INCAR |-.HHSs-POTCAR |-.a-[CaAs]1en ->POTCAR …… |-.Output-data |- Formation-energy_bandgap_information.docx |-Relaxed_structure_information.xlsx We expect this database will serve as a valuable resource for the scientific community to further explore the tetrahedral-bonding hybrid heterostructured semiconductors