The Hazelett continuous casting and rolling process represents a leading-edge production method for cold-rolled aluminum sheet and strip billets in the world. Its solidification microstructure significantly influences the quality of billets produced for cold rolling of aluminum sheets and strips. In this study, employing the CAFE (Cellular Automaton—Finite Element) method, we developed a coupled computational model to simulate the solidification microstructure in the Hazelett continuous casting process. We investigated the impact of nucleation parameters, casting temperature, and continuous casting speed on the microstructural evolution of the continuous casting billet. Through integrated metallographic analyses, we aimed to elucidate the controlling mechanisms underlying the Hazelett continuous casting process and its resultant microstructure. The results demonstrate that the equiaxed rate of grains increases with an increase in nucleation density, and the grain size decreases under constant cooling strength. With other nucleation parameters held constant, the grain size decreases as undercooling increases, and the columnar crystal zone expands. The nucleation density of the Hazelett continuous casting aluminum alloy has been determined to range between 1011 m−3 and 1013 m−3, and the undercooling ranges between 1 °C and 2.5 °C. The solidified grain structure can be controlled between 35 μm and 72 μm. The grain size of the continuous casting billet increases with an increase in pouring temperature and decreases as the casting speed increases. Elevating the pouring temperature positively impacts the fraction of high-angle grain boundaries and promotes the dendritic to equiaxed grain transition. Moreover, there exists potential for further optimization of continuous casting process parameters.