Herein, we assess the quality of SpaiNN predictions using two classes of model systems: Firstly, we delve into the light-induced rotation around a double bond across a series of alkenes: ethene (C 2 H 4 ), propene (C 3 H 6 ), and butene (C 4 H 8 ). To achieve this, we created the XALKENEDB database at the complete active space self-consistent field (CASSCF) level of theory , specifically averaging the three lowest singlet states targeting two active electrons distributed over two active orbitals, denoted as SA(3)-CASSCF (2,2). A total number of circa 6 k (for C 2 H 4 and C 3 H 6 each) and 13 k (C 4 H 8 ) reference calculations were performed for the respective alkenes, from which the following five quantum chemical features are stored in the XALKENEDB database: energies, forces, NACs, and dipole moment vectors (comprising both permanent and transition dipole moment vectors). Detailed information regarding the construction of the XALKENEDB database is provided in the Supporting Information (cf. section S2).