The VIB5 database is a meticulously curated collection of high-quality ab initio quantum chemical data for five small polyatomic molecules with significant astrophysical relevance: methyl chloride (CH 3 Cl), methane (CH 4 ), silane (SiH 4 ), fluoromethane (CH 3 F), and sodium hydroxide (NaOH). The database includes over 300,000 grid points, with individual molecules featuring between 15,000 and 100,000 points. Each grid point corresponds to a specific nuclear configuration of the molecule, providing theoretical best estimates (TBEs) of potential energies and their constituent terms. Additionally, the data set offers energy and energy gradient calculations at various levels of theory, including MP2/cc-pVTZ and CCSD(T)/cc-pVQZ, as well as HF energies derived from these calculations using the corresponding basis sets.