Crystalline hydroxyapatite (HA) and 0.8 wt.% silicon-substituted HA (SiHA) thin films were produced using magnetron co-sputtering. These films were subjected to contact angle measurements and in vitro cell culture study using human osteoblast-like (HOB) cells. A wettability study showed that SiHA has a lower contact angle, and thus is more hydrophilic in nature, as compared to HA. Consequently, enhanced cell growth was observed on SiHA at all time-points. Furthermore, distinct and well-developed actin filaments could be seen within HOB cells on SiHA. Thus, this work demonstrated that the surface properties of the coating may be modified by the substitution of Si into the HA structure.