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Plasma alloying technique capable of producing metallic coatings with metallurgical bonding has attracted much attention in dental and orthopedic fields. In this study, the effects of temperature and time of plasma tantalum (Ta) alloying technique on the mechanical, electrochemical, and osteoblastic properties of Ta coatings were systematically investigated. Ta coatings prepared at 800 °C possess better interfacial strengths than those prepared at 750 and 850 °C, and the interfacial strength increases with prolonged alloying time (30–120 min). At 800 °C, however, the increased proportion of the soft Ta deposition layer with alloying time in the whole coating impairs the surface mechanical properties of the entire coating, as convinced by decreased microhardness and wear resistance. Moreover, Ta coatings exhibit better corrosion resistance than the Ti6Al4V substrate in Dulbecco’s modified Eagle medium. The enhanced adhesion and extracellular matrix mineralization level of osteoblasts demonstrate the better cytocompatibility and osteogenic activity of the Ta coating. Ta30 (Ta coating prepared at 800 °C for 30 min) exhibits excellent mechanical, electrochemical, and osteoblastic behaviors and is promising in biomedical applications.