<p>The mechanical strength and biocompatibility of the Ti-15Mo-5Zr-3Al (Ti1553) alloy make it a promising material for orthopaedic implants. However, its limited bioactivity and antibacterial performance hinder its clinical applications. Herein, a novel Ca²⁺ decorated nanostructured titanate coating was developed on the surface of Ti1553 using successive NaOH treatment, calcium nitrate modification, and heat treatment. Among all the samples and treatments, 100 mM Ca-treated Ti1553 alloy exhibited higher calcium incorporation (~ 1.7 at%) and a significant reduction in contact angle (~ 9°), indicating improved hydrophilicity and surface energy. Raman and XRD analyses confirmed the formation of calcium titanate and hydroxyapatite-like phases on the modified surface. The Ca²⁺ modified Ti1553 exhibited superior apatite precipitation, indicating enhanced bioactivity in simulated body fluid. Ca²⁺ ion incorporation also facilitates apatite deposition, which will contribute to the bonding of bone to the implant. The strong antibacterial activity was also observed with the zone of inhibition (18.5 ± 1.2&#xa0;mm). The sample also demonstrated the improved protein adsorption (~ 2-fold) and osteoblast adhesion due to the Ca²⁺ enrichment on the surface. These findings on Ca²⁺ decorated titanate coating shows that the 100 mM Ca-treated Ti1553 alloy is the favourable candidate for the orthopaedic and dental applications.</p> Graphical Abstract <p></p>