Present article provides a method of Bi@SiO2 core@shell nanocomposites obtaining via surface modification of laser-synthesized bismuth nanoparticles with tetraethoxysilane.The SiO2 shell coating on Bi nanoparticles was demonstrated to form spherical nanoformulations with the mode of size distribution at 250–300 nm. The developed approach is a novel perspective alternative to the traditional methods that allows designing biocompatible Bi-based nanocomposites for the sensitization of multimodal theranostics.