The fatigue strength of high silicon-alloyed nodular cast iron is influenced by casting defects and graphite precipitates. The literature as well as the findings of this work show that these microstructural constituents can be tailored by controlling silicon microsegregation. In addition, segregations also affect the ferritic matrix microstructure locally. In the present work, silicon segregations in high silicon-alloyed ductile iron are specifically manipulated by small additions of aluminum. It was demonstrated how the aluminum content affects a wide range of microstructural constituents across a variety of length scales. Specimens from alloys with small additions of aluminum were fabricated and tested by rotating bending. Results show that the fatigue strength can be increased compared to a reference alloy with no aluminum. Microstructure analysis as well as fractography were performed concluding that microstructural changes could be attributed to the increased aluminum content, which allows the fatigue properties to be tailored deliberately. However, according to the results of this study, the negative effect of aluminum on castability and graphite morphology limits the maximum content to approximately 0.2 wt.%.