Calcium hydroxide cements can lack long-term stability and achieve sustained release by matrix-controlled diffusion of hydroxyl ions. Tetracalcium phosphate (TTCP) hydrolyzes slowly to form calcium hydroxide and a thin insoluble apatite layer that prevents further reaction. In this study, mechanical amorphization was used to create a setting calcium-hydroxide-releasing cement from TTCP. The effect of high-energy ball milling of TTCP on the mechanical properties of the cement was investigated. X-ray diffraction data were used to determine the phase composition of the set cements. An accelerated in vitro test compared pH of water after prolonged boiling of nanocrystalline TTCP cements and a calcium salicylate material. As milling time increased, cement compressive strength and degree of conversion increased. Hydroxyl ion release from the cement was comparable with that from a calcium salicylate material. This new cement system offers the antimicrobial potential of calcium salicylate materials combined with the long-term stability of insoluble apatite cements.