Computational Methodology: The xxMD data set includes four photochemically active molecular systems: azobenzene, malonaldehyde, stilbene, and dithiophene. To investigate the complex electronic structures involved in these systems, particularly in the vicinity of deformed geometries and conical intersections, nonadiabatic simulations were performed using the trajectory surface hopping algorithm implemented in the SHARC code. The state-averaged complete active space self-consistent field (SA-CASSCF) level of theory was employed to accurately describe the potential energy surfaces of the multiple electronic states relevant to these systems. This subset of data, generated from SA-CASSCF calculations, is referred to as xxMD-CASSCF. The trajectories in xxMD-CASSCF exhibit energy conservation and provide potential energies and forces for the first three electronic states. All SA-CASSCF calculations were carried out using OpenMolcas 22.06. To ensure compatibility with existing data sets (MD17 and rMD17), a new subset xxMD-DFT is created which provides recomputed ground singlet electronic state potential energies and gradients using spin-polarized KS-DFT calculations with the M06 functional for the same geometries as used in SA-CASSCF calculations. All calculations are done with the Psi4 package interfaced with ASE package. It should be noted that the xxMD data set does not include nonadiabatic coupling vectors (NACs) for reasons described in their reference data descriptor.