Spherical sheet steel molds filled with gray iron melts of varying chemical compositions and metallurgical conditions were air-cooled until solid, followed directly by austempering to preserve the austenite grain structure. The castings were studied using a combination of cooling curves and quantitative metallography, in order to clarify control of the austenite grain structure and its impact on the local microstructure. A novel method utilizing fast Fourier transform provided visual overview of macroscopic trends in the scale of the flake graphite structure. Castings inoculated with Sr-containing ferrosilicon featured finer eutectic cell structure but coarser equiaxed structure of austenite, emphasizing that melt treatments applied to control the graphite structure may have unintended effects on the austenite grain structure. In most non-inoculated castings, the microstructure was banded, with alternating layers of coarse and fine flake graphite with distance from the casting surface. The extent of the columnar zone of austenite grains showed no correlation with the graphite structure nor the volume fraction of dendrites. The volume-to-surface ratio of dendrites was more uniform in the columnar zone, but increased toward the center in the equiaxed zone. The casting with the highest carbon equivalent (4.34), featured zones containing finer dendrites and graphite. These zones appear to be gaps in the early solidification structure which filled later by secondary dendritic growth from surrounding austenite. This highlights that high carbon equivalent may lead to poor dendrite coherency which can make the microstructure less uniform and less predictable.