Figure illustrates the large chemical diversity of the TM-GSspin dataset, encompassing various metal identities, OS, coordination geometries, as well as compositions of the first coordination sphere. Each metal exhibits three OSs, with a number of d electrons ranging from 3 to 8 (Figure ). Seventeen types of coordination geometries are obtained, with coordination numbers ranging from 2 to 8 (Figure ). Those include common geometries like octahedral, tetrahedral, or square planar, as well as less common ones such as linear, trigonal planar, pentagonal bipyramidal, or capped trigonal prismatic. Nitrogen is found to be the most recurrent metal-coordinating atoms followed by oxygen, carbon, sulfur, phosphorus, chlorine, and bromine (Figure ). Combinations of different metal-coordinating elements across various coordination numbers and geometries lead to over 600 different first coordination spheres, including complexes with up to 5 different coordinating elements (Figure ). In comparison with the original database 22 of 15,837 complexes mined from the CSD, the TM-GSspin dataset is characterized by an increased proportion of complexes with less common coordination geometries (e.g., the proportion of trigonal planar complexes increases from 0.7 % in the original database to 2.7 % in the TM-GSspin dataset) and those with zero or low-valent OSs (see comparison in Figure in the SI).