In this work, a simple, green, and transition metal-free approach to the N-arylation of secondary amines with aryl halides in magnetized distilled water (MDW), as a solvent, is introduced. This method offers the advantages of short reaction times, low costs, and an additive-free process, and it also enables new planning strategies for the construction of aryl amine-containing pharmacophores. Also, the reaction rates were followed spectrophotometrically by monitoring the changes in the absorption spectrum of the reaction mixture in ordinary and magnetized distilled water. Furthermore, we used the reliable molecular dynamics (MD) simulations as predictive tools to interpret and describe the interactions between reactants in the ordinary and magnetized distilled water. The RDFs analysis of interactions revealed that morpholine and iodobenzene reactants were surrounded by more solvents in MDW than ordinary distilled water (ODW) 90 °C. Consequently, the high reactivity observed for two reactants in MDW at 90 °C can be explained by MD simulation, and there comes an established synergy between the theoretical calculation and experiment.