In order to achieve high-efficiency perovskite solar cells, understanding both the crystal structure and the optoelectronic properties of perovskite layers is of importance. This paper uses crystallization analysis and the modeling study of two different perovskite deposition methods (two- and one-step methods) and thereby shows that the one-step method embodies a film formation process that is dominated by crystal growth, while the dominant mechanism of the two-step procedure is nucleation. Our data based on experimental and theory shows that the one-step recipe is superior in terms of morphology control, and, hence, reproducibility, compared to the two-step recipe.