The uncontrollable rapid degradation rate of the Mg alloy substrate limited its clinical application, and implant-associated infections have been reported to be the main reason for the secondary surgery of orthopedic implantation. The aim of this study was to produce a multifunctional coating on magnesium-based alloys that have improved corrosion resistance, bioactivity, and antibacterial properties through the preparation of polyelectrolytic multilayers (PEMs) consisting of chitosan (CS) and sodium hyaluronate (HA) on silane-modified strontium-substituted hydroxyapatite (hereafter referred to as Bil (SH + CS)/SrHA). The multifunctional coatings were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), and X-ray photoelectron spectroscopy (XPS). The results showed the polyelectrolyte complex SH/CS layer to be uniformly and tightly attached on to the surface of silane-treated SrHA. At the same time, a potentiodynamic polarization test and hydrogen evolution test showed the Bil (SH + CS)/SrHA coatings to exhibit superior corrosion resistance than bulk Mg-based alloys. The results of the cell–surface interactions revealed Bil (SH + CS)/SrHA coatings to be in favor of cell initial adhesion and more beneficial to the proliferation and growth of cells with the processing of co-culture. In addition, antibacterial tests demonstrated the strong bactericidal effect of Bil (SH + CS)/SrHA coatings against both Escherichia coli (E. coli) and Staphylococcus (S. aureus), suggesting that Bil (SH + CS)/SrHA coatings can successfully achieve multifunctionality with enhanced corrosion resistance, biocompatibility, and antibacterial properties.