In this study, the in-vitro bone regeneration ability of commercial pure titanium (CP-Ti) surface modified via electrospun polyvinylidene/hydroxyapatite (PVP/HA) masking and subsequent Nd-YAG pulsed laser treatment was investigated. The ratio of HA to PVP played a significant role in achieving a perfect homogenous mask on the CP-Ti. In the laser treatment process, the parameter of area scanning speed (ASS) had an important influence on the final surface morphology. A favorable range was defined for this parameter where these two conditions were satisfied: no PVP remaining and no severe substrate melting. Within a favorable range of ASS, as decreasing ASS exchanged the surface structure from detached particles to a pattern-like network. The calcium titanate CaTiO3 (CTO) and α-tricalcium phosphate (α-TCP) were formed as the main components on the CP-Ti surface. The coating had an adequate adhesion to the CP-Ti surface. Furthermore, a surface with a water affinity between hydrophilic and hydrophobic was obtained. The in-vitro bioactivity test revealed that the surface modification enhanced the bone-like apatite formation. The cytocompatibility assays confirmed that the cell attachment and spreading of the osteosarcoma-like cells (MG63) were improved by the surface treatment. The development of surface modification techniques opens new avenues in bone tissue engineering applications.