This study reports preparation and characterization of biocompatible, conductive, and flexible silk-Pt composite materials for applications in wearable and medical devices. The distinct Pt and silk materials were integrated via supercritical carbon dioxide (sc-CO2) promoted electroless plating. Sc-CO2 was introduced into the catalyzation step, which is a critical step in electroless plating, to overcome the common difficulty of inlaying the catalyst into the textile substrate. High surface coverage and thick Pt layer were constructed as the metallization time extended. Metal ions released in a simulated body fluid in an immersion test were negligible when compared to the daily metal input and output of the human body. The composites showed high corrosion resistances in both 3.5 wt % NaCl and simulated body fluid solutions. The electrical conductivity and corrosion resistance persisted after the adhesion tests. The assessments revealed the applicability of this silk-Pt material to wearable and medical devices.