Encapsulation of gold nanoparticles within a silica shell is highly beneficial to the preparation of highly concentrated gold nanoparticles that can strongly absorb X-ray and hence be used as an X-ray contrast agent. This chapter describes a method for preparing highly concentrated colloidal gold nanoparticles suitable for an X-ray contrast agent application. It describes specific details of procedures for preparing spherical gold nanoparticles, forming thin silica shell on each gold nanoparticle, and enriching the silica-encapsulated gold nanoparticles.