Potassium and sodium containing nanoapatite cements were produced from Ca2KNa(PO4)2 by prolonged high energy ball milling of the compound for up to 24 h. This mechanical treatment resulted in the decrease of the crystal size and a partial amorphisation of the cement reactant as shown by X-ray diffraction analysis and the appearance of strong exothermic peaks in differential scanning calorimetry measurements. The pH of water saturated with Ca2KNa(PO4)2 was 12.5 when the material was mechanically activated but was only 9.5 for the untreated compound suggesting an increase in solubility following milling. The cements set following mixing with a 2.5% Na2HPO4 solution in clinically acceptable times between 5-12 min and showed compressive strengths of up to 11 MPa after 24 h setting. The strong alkaline pH value of the cements may provide antimicrobial potential for an application in dentistry as pulp capping agents or cavity liners or for the treatment of infected bone sites.