Strategies involving the synthesis of hydroxyapatite (HAP) are significant in health and materials sciences, and lately, in heritage science. Conditions for the optimized heterogeneous formation of HAP for consolidating bone are investigated using a simple methodology with discs of calcium-containing starting materials and phosphate-containing reagent solutions; the results were evaluated against whole bone specimens. Diammonium phosphate (DAP) solutions with simulated body fluid (SBF) and gelatin as cofactors in all combinations were used in trials, while the products were characterized by microscopy, elemental microanalysis, X-Ray diffractometry, and Fourier transform infrared spectroscopy. The hypothesis that bone, SBF, and gelatin may biomimetically promote HAP formation was tested through a simple experimental design. The results showed that HAP is generally formed in mixtures with octacalcium phosphate (OCP), as well as calcium hydrogen phosphate dihydrate (brushite). The precipitation of carbonate HAP signals the formation of a biocompatible product in the cases where SBF and gelatin were employed as cofactors. Gelatin was found to further promote the product formation in most cases. It was shown that DAP, as well as its combination with gelatin, could predominantly form HAP in most trials, while OCP is co-crystallized in SBF-containing solutions.