The current experimental investigation in this article was designed to characterize the structure of mold (M) and ladle (L) inoculated, low-S (0.025 wt.% S), low-Al (0.003 wt.% Al), slightly hypereutectic (CE = 4.4-4.5 wt.%) electric melted gray irons, typical for high performance thin-wall castings. It describes the effect of a Ca, Al, Zr-FeSi inoculant addition of 0-0.25 wt.% on structure characteristics, and compares to similar treatments with hypoeutectic irons (3.5-3.6 wt.% CE, 0.025 wt.% S, and 0.003 wt.% Al). A complex structure including primary graphite, austenite dendrites, and eutectic cells is obtained in hypereutectic irons, as the result of nonequilibrium solidification following the concept of a coexisting region. Dendrites appear to be distributed between eutectic cells at higher eutectic undercooling, while in inoculated irons and for lower undercooling, the eutectic cells are “reinforced” by eutectic austenite dendrites. A Zr, Ca, Al-FeSi alloy appears to be an effective inoculant in low S, low Al, gray cast irons, especially for a late inoculation technique, with beneficial effects on both graphite and austenite phases. First, inoculation influenced the nucleation of graphite/eutectic cell, and then their characteristics. A further role of these active elements directly contributed to form nucleation sites for austenite, as complex (Mn,X)S particles.