Due to the gradual shift to less rich iron ores, the alumina content in the raw materials used for iron-making is progressively increasing, affecting the mineralogy and the properties of iron ore sinters. In this context, the effect of Al content on the mechanical properties of calcium aluminosilicoferrites Ca2(Ca,Mg,Fe)6(Fe,Si,Al)6O20 (SFCA), which is the most important bonding phase in iron ore sinters, is of particular interest. In this study, high-alumina calcium aluminosilicoferrites were synthesized and their mechanical properties were determined by nanoindentation using a cube-corner indenter. For synthesis, different raw materials were taken as proxies for the adhering layer in a sinter granule. Three mixtures were prepared, high-iron, high-silica, and high-alumina and heated in an alumina crucible, which was used to simulate the high-alumina nucleus in a granule. The different raw materials used for synthesis had only minor influence on the compositions of the synthesized ferrites. All ferrites showed similar mechanical behavior during indentation, indicating that neither the chemical nor the mechanical properties were affected by the different compositions of the adhering layer, when the sinter granule is dominated by a high-alumina nucleus. The crystallographic orientation of the tested grains had only minor influence on the results of the nanoindentation experiments.