The dataset consists of energies and forces for pristine and defected monolayer graphene, bilayer graphene, and graphite in various states. The configurations in the dataset are generated in two ways: (1) crystals with distortions (compression and stretching of the simulation cell together with random perturbations of atoms), and (2) configura- tions drawn from ab initio molecular dynamics (AIMD) trajectories at 300, 900, and 1500 K. For monolayer graphene, the configurations include: * pristine - In-plane compressed and stretched monolayers - AIMD trajectories * defected - Configurations from the minimization of a monolayer with a single vacancy - AIMD trajectories of monolayers with a single vacancy For bilayer graphene, the configurations include: * pristine - AB-stacked bilayers with compression and stretching in the basal plane - Bilayers with different translational registry (e.g. AA, AB, and SP) at various layer separations - Twisted bilayers with different twisting angles at various layer separations - AIMD trajectories of twisted bilayers and bilayers in AB and AA stackings * defected - Configurations from