Thiol-modified poly(ethylene glycol) (mPEG-SH) has been used to replace standard capping agents from the surfaces of gold nanoparticles with different sizes and shapes. Upon PEG stabilization, the nanoparticles can be transferred into ethanol, where silica can be directly grown on the particle surfaces through the standard Stober process. The obtained silica shells are uniform and homogeneous, and the method allows a high degree of control over shell thickness for any particle size and shape. Additionally, Raman-active molecules can be readily incorporated within the composite nanoparticles during silica growth so that SERS/SERRS-encoded nanoparticles can be fabricated containing a variety of tags, thereby envisaging multiplexing capability.