Coral reefs face unprecedented threats from climate change and human activities, making reef restoration increasingly important for the preservation of marine biodiversity and the sustainability of coastal communities. One promising restoration method relies on coral breeding and larval settlement, but this approach requires further innovation to achieve high rates of settlement and survival. In this study, we built on our previous work engineering lime mortar-based coral settlement substrates by investigating three different compositions of a natural hydraulic lime (NHL) base material as well as composite NHL substrates containing alkaline earth metals. These materials were tested with larvae of three reef-building Caribbean coral species: Orbicella faveolata (Mountainous star coral), Diploria labyrinthiformis (Grooved brain coral), and Colpophyllia natans (Boulder brain coral). We found that the base material composition, including its silicate and calcium carbonate (CaCO3) content, as well as the addition of the inorganic additives strontium carbonate (SrCO3), magnesium carbonate (MgCO3), and magnesium sulfate (MgSO4), all influenced coral larval settlement rates. Overall, NHL formulations with lower concentrations of silicate and higher concentrations of calcium, strontium, and magnesium carbonates significantly increased coral settlement. Further, when dissolved ions of magnesium and strontium were added to seawater, both had a significant effect on larval motility, with magnesium promoting settlement and metamorphosis in C. natans larvae, supporting the observation that these additives are also bioactive when incorporated into substrates. Our results demonstrate the potential benefits of incorporating specific inorganic ion additives such as Mg2+ and Sr2+ into substrates to facilitate early coral life history processes including settlement and metamorphosis. Further, our results highlight the importance of optimizing multiple aspects of coral substrate design, including material composition, to promote settlement and survival in coral propagation and reef restoration.