This dataset supports the results included in the poster presentation ‘Molecular Dynamics of Paramagnetic and Water in Hydrates’, Arifah Abdu Rahaman, DA Faux, PJ McDonald, at the 39th Cement and Concrete Science Conference, 9-10 September 2019, University of Bath, UK. NMR is an important technique for non-destructively characterising cement materials. NMR relaxation rate response is dominated by the interactions of water with paramagnetic ions. This research aims to inform a simplified theoretical model in order to interpret the experimental data. The results of molecular dynamics (MD) simulations are presented to describe the nano-scale dynamics of the paramagnetic impurities and the water. The model will contribute to the interpretation of NMR results from cement-like material such as cement paste, plasters and mortar. The results proved that the key physics behind the theoretical model are well captured to describe the nano-scale dynamics of the paramagnetic impurities and the water. In future, the model will predict the frequency dependent spinlattice relaxation time T1 (f) for a range of aqueous paramagnetic ions to provide fits to experimental data. The conference proceedings are published by University of Bath in association with Cementitious Materials Group, Institute of Materials Minerals and Mining, London, UK. https://researchportal.bath.ac.uk/en/publications/39th-cement-and-concrete-science-conference-2019 https://purehost.bath.ac.uk/ws/portalfiles/portal/197842011/39th_Cement_and_Concrete_Science_Conference_2019.pdf