Using the commercial finite element software ProCAST to predict the temperature field, the flow field, the turbulent kinetic energy, and melt-pool outlet temperature of the top side-pouring twin-roll casting (TSTRC) of 6.5 wt.% Si steel process, and the cellular automaton–finite element (CA-FE) method was used to simulate the melt-pool outlet microstructure. The effect of different process conditions on the TSTRC process was investigated through numerical simulation and a processing technic appropriate for the production of 6.5 wt.% Si steel was obtained. Meanwhile, the influence of violent stirring in the melt-pool on the microstructure under different process conditions was evaluated. It was found that vigorous stirring in the melt-pool was conducive to formate the equiaxed crystal structure. Not only realized the near-final shape of the metal sheet, but also realized the near-final shape of the microstructure. Chose the proper process to experiment, and from comparing the simulation and the experiment, the simulation and experimental results were in good agreement, which verified the simulation's feasibility and accuracy.