The surface treatment of titanium implants has been applied mainly to increase surface bioactivity and, more recently, to introduce antibacterial properties. To this end, composite coatings have been investigated, particularly those based on hydroxyapatite. The present research was aimed at the development of another coating type, chitosan–nanosilver, deposited on a Ti13Zr13Nb alloy. The research comprised characterization of the coating’s microstructure and morphology, time-dependent nanosilver dissolution in simulated body fluid, and investigation of the nanomechanical properties of surface coatings composed of chitosan and nanosilver, with or without a surface-active substance, deposited at different voltages for 1 min on a nanotubular TiO2 layer. The microstructure, morphology, topography, and phase composition were examined, and the silver dissolution rate in simulated body fluid, nanoscale mechanical properties, and water contact angle were measured. The voltage value significantly influenced surface roughness. All specimens possessed high biocompatibility. The highest and best adhesion of the coatings was observed in the absence of a surface-active substance. Silver dissolution caused the appearance of silver ions in solution at levels effective against bacteria and below the upper safe limit value.