Two benchmark datasets, comprising 22 well-known supramolecular cages, have been selected from the supramolecular chemistry literature to evaluate cavity detection and volume characterization. All supramolecular cage structures were prepared in the following way: the original CIF files were downloaded from the Cambridge Structural Database (CSD) and atoms and molecular fragments, that are not part of the cage-framework, were removed from the structures, using Diamond Crystal and Molecular Structure Visualization software and saved in a PDB format. Benchmark dataset 1: host-guest pairs For benchmark dataset 1, the guest structures were obtained, from the corresponding CIF files, by removing the supramolecular cage and other molecular fragments that are not part of the guest. Supramolecular Cage Identifier Guest CSD Identifier DOI B1 Et4N+ 718468 10.1021/ic8012848 B2 BnNMe3+ 718469 10.1021/ic8012848 B3 (Cp)2Co+ 718470 10.1021/ic8012848 B4 (Cp*)2Co+ 718471 10.1021/ic8012848 B5 BF4- 1862753 10.1002/asia.201801262 B6 ClO4- 1862752 10.1002/asia.201801262 B7 C60 942782 10.1021/ja4110446 B8 C60 1872778 10.1002/chem.201805353 B9 Adamantane-2,6-dione 183906 10.1002/1521-3757(20021018)114:203.0.CO;2-X B10 Et4N+ 100947 10.1002/(SICI)1521-3773(19980803)37:13/143.0.CO;2-D B11 Corannulene and Cyclohexane 2068665 10.1038/s41467-021-24344-w B12 C60 2068666 10.1038/s41467-021-24344-w B13 C70 2068667 10.1038/s41467-021-24344-w Benchmark dataset 2: topologically and morphologically distinct supramolecular cages The single resorcin[4]arene ligand (O2) was prepared from the corresponding resorcin[4]arene-cage (A1) by removing 5 ligands. In the cyclotricatechylene cage (C1), the outward-pointing phenyl groups (that do not affect the cavity calculations) were removed. Supramolecular Cage Identifier CSD Identifier DOI A1 1207879 10.1038/38985 C1 1892128 10.1039/C9CC02103E F1 293777 10.1126/science.1124985 F2 1831430 10.1038/nature20771 H1 768969 10.1039/C0CC00234H N1 1541839 10.1021/jacs.7b05202 O1 2074472 10.1021/acs.joc.1c00794 O2 1207879 10.1038/38985 W1 1416694 10.1038/nchem.2452