Zinc chloroapatite (ZnClAp), a promising material for bone treatment, was synthesized by a mechanochemical method. The effect of synthesis condition on its crystallinity was investigated. Starting materials (i.e., calcium monohydrogen phosphate dihydrate, calcium oxide, zinc oxide and calcium chloride) were kneaded with water at four kinds of water/solid ratios in a planetary ball-mill. Thus obtained products were analyzed by a powder X-ray diffractometry (PXRD) and an attenuated total reflection -infrared (ATR-IR) spectroscopy. The PXRD and ATR-IR results indicate that ZnClAp has successfully been synthesized by the present method. PXRD results indicate that the crystallinity of ZnClAp increases with the water/solid ratio of the kneaded paste for the synthesis. This finding is supported by a principal component analysis (PCA) that is applied to the ATR-IR spectra. The present mechanochemical method is simple, economy, and is useful for the synthesis of ZnClAp.