Pseudowollastonite (CaSiO3) coatings on titanium alloy substrates were prepared by laser ablation. The in vitro bioactivity of the coatings was examined for its biomedical applicability which was evaluated by immersion in human parotid saliva. The pseudowollastonite-coatings were soaked for various periods and characterized by SEM-EDS, XRD, FTIR, and TEM analysis, and the results indicated that the carbonated hydroxyapatite (CHA) was formed on the surface of the coatings within 1 day. In addition, cell attachment test showed that the pseudowollastonite-coatings supported the mesenchymal stem cells adhesion and spreading, and the cells established close contacts with the ceramics after 1 day of culture. These findings indicate that the pseudowollastonite-coatings possesses good bioactivity, biocompatibility and could be of interest in specific periodontal applications for bone restorative purposes.