Data Accessibility: COMPAS datasets are publicly available at where molecules and their corresponding QM properties including electronic energies, HOMO/LUMO energies and gap, ZPE, etc., are hosted. An online website is developed for easier structure search and download at . 3.33 CREMP CREMP (Conformer-Rotamer Ensembles of Macrocyclic Peptides) data set aims to explore macrocyclic peptides which is lacking in MLP field, providing 36k representative 4-, 5-, and 6-mer homodetic cyclic peptides with up to 31.3 million unique conformers with properties calculated at semiempirical level. CREMP-CycPeptMPDB data set is also provided which is built based on the established CycPeptMPDB database featuring passive membrane permeability with 8.7 million newly-generated conformers from 3k 6-, 7-, and 10-mer cyclic peptides.