The paper reports on a freeze-granulation technique to prepare a novel nanocomposite of poly(methyl methacrylate) (PMMA)-modified hydrodyapatite (HA) with multiwalled carbon nanotubes (MWCNTs) as reinforcement for a new generation biomedical bone cement and implant coatings. By using this technique it is possible to increase material homogeneity and also enhance the dispersion of MWCNTs in the composite matrix. The phase composition and the surface morphology of the nanocomposite material were studied using X-ray diffraction, field-emission scanning electron microscopy, and micro-Raman spectroscopy. Additionally, nanomechanical properties of different concentrations of MWCNT-reinforced nanocomposite were performed by a nanoindentation technique, which indicates that a concentration of 0.1 wt% MWCNTs in the PMMA/HA nanocomposite material gives the best mechanical properties.