A program was conducted to research how to characterize the size and shape of micro-particles. These can act as graphite nuclei, but are altered by adding a commercial iron powder, or after a similar treatment combined with inoculation. Resin sand mold (RSM) and metal mold (MM) solidified sample structures were subjected to automatic image analysis. In general, a higher cooling rate, typical for MM solidification, favors smaller size and more compact particles, even in RSM media. Iron powder treatment led to the largest particles with unusual morphologies, better defined by complex shape factors, which employ actual perimeters, rather than the simpler median size and aspect ratio method. Conventional inoculation employed after an iron powder treatment altered the particles (smaller and more compact), which benefited their effectiveness to act as graphite nuclei, especially at slower solidification rates in RSMs. The results confirm that promoting more compact micro-inclusions, at smaller sizes, involved in graphite nucleation, reduces the sensitivity to chill and improves the eutectic cell characteristics in gray cast iron.