In the current study, a mathematical formulation is developed by combining the non‐Newtonian (Casson) fluid model to simulate the thermosolutal free convection radiative flow over a vertical surface. The current flow model is formulated with a heat sink/source and radiation driven by Arrhenius kinetics. The basic flow equations are transmuted into a nondimensional form via similarity transformations for which numerical simulations are performed utilizing the Runge‐Kutta‐Fehlberg method with shooting technique. The results obtained for velocity, energy, and species mass concerning various flow parameters are presented graphically. Computed results for skin friction, Nusselt number, and Sherwood number are tabulated. The results have been verified for limited cases by comparing with various investigations, revealing excellent accuracy. The detailed geometry reveals that an increase in the activation energy enhances the flow velocity and heat transport in the Casson fluid system due to exothermic heat reaction. With the increase of the Frank‐Kamenetskii term, there is a substantial rise in temperature distribution and a decrease in concentration profiles due to high Arrhenius exothermic process, which revealed that the presence of Arrhenius kinetics is more effective to improve heat transportation phenomenon. Enhancement of the heat source/sink term completely boosts heat distribution. Rise in Radiation parameter, temperature field increases by reducing heat dissipation to the ambient.