A β-Ta nanocrystalline coating was engineered onto a Ti-6Al-4V substrate using a double cathode glow discharge technique to improve the corrosion resistance and bioactivity of this biomedical alloy. The new coating has a thickness of~40 µm and exhibits a compact and homogeneous structure composed of equiaxed β-Ta grains with an average grain size of~22 nm, which is well adhered on the substrate. Nanoindentation and scratch tests indicated that the β-Ta coating exhibited high hardness combined with good resistance to contact damage. The electrochemical behavior of the new coating was systematically investigated in Hank's physiological solution at 37 • C. The results showed that the β-Ta coating exhibited a superior corrosion resistance as compared to uncoated Ti-6Al-4V and commercially pure tantalum, which was attributed to a stable passive film formed on the β-Ta coating. The in vitro bioactivity was studied by evaluating the apatite-forming capability of the coating after seven days of immersion in Hank's physiological solution. The β-Ta coating showed a higher apatite-forming ability than both uncoated Ti-6Al-4V and commercially pure Ta, suggesting that the β-Ta coating has the potential to enhance functionality and increase longevity of orthopaedic implants.