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Biocompatibility of HEAs in the TiZrHfNbTa system in which all the constituents are non-toxic and allergy-free was scrutinized systematically, and novel biomechanical materials with a unique combination of low modulus (57 GPa, almost half that of conventional biomedical titanium alloys), good mechanical biocompatibility and low magnetic susceptibility (1.71 × 10⁻⁶ cm³ g⁻¹, similar to that of pure Zr) were successfully developed. Moreover, the underlying mechanisms responsible for phase formation and promising properties were explored. This work not only offers a series of novel bio-metallic materials with prominent properties for practical applications, but also shed light on understanding of phase formation and strengthening of HEAs in general.