Ti-24Nd-4Zr-7.9Sn alloy with low elastic modulus and high strength is a great candidate for artificial biomaterials used in orthopedic and dental implants. In order to improve biocompatibility, a biomimetic process was employed to deposit a bone-like apatite nanocrystal coating on alloy. Analysis of the coatings showed that a net-like Na2TiO3 layer with about 100 nm in size was formed on Ti-24Nd-4Zr-7.9Sn treated by NaOH. Consequently, a carbonated apatite nanocrystal coating, namely bone-like apatite, was biomimetically deposited on Na2TiO3 layer, which has similar mineral composition to that of natural bone. The growth mechanism of bone-like layer is also discussed.