The surface of titanium (Ti) dental implants must be modified to improve their applicability, owing to the biological inertness of Ti. This study aims to use sandblasting as a pretreatment method and prepare a hydroxyapatite (HA) coating on Ti to improve its biocompatibility and induce bone bonding and osteogenesis. In this paper, sandblasted Ti discs were coated with α-tricalcium phosphate (α-TCP) via Er:YAG pulsed laser deposition (Er:YAG-PLD). An HA coating was then obtained via the hydrothermal treatment of the discs at 90 °C for 10 h. The surface characteristics of the samples were evaluated by SEM, SPM, XPS, XRD, FTIR, and tensile tests. Rat bone marrow mesenchymal stem cells were seeded on the HA-coated discs to determine cellular responses in vitro. The surface characterization results indicated the successful transformation of the HA coating with a nanorod-like morphology, and its surface roughness increased. In vitro experiments revealed increased cell attachment on the HA-coated discs, as did the cell morphology of fluorescence staining and SEM analysis; in contrast, there was no increase in cell proliferation. This study confirms that Er:YAG-PLD could be used as an implant surface-modification technique to prepare HA coatings with a nanorod-like morphology on Ti discs.