This work describes a method to decorate carbon nanotubes (CNTs) with metallic Pd and Ru nanocrystals via inorganic reactions in supercritical (SC) CO2-methanol solutions. In this route, PdCl2 or RuCl3.3H2O dissolved in SC CO2-methanol solution acted as a metal precursor and CNTs functioned as a template to direct the deposition of produced nanoparticles. Methanol served as the reductant for the precursors as well as cosolvent to enhance the dissolution of precursors in SC CO2. Dry products were readily obtained through in situ extraction with SC CO2 after reactions. The products were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy. It was demonstrated that the loading content and particle size of the nanoparticles deposited on CNTs could be tuned by changing the weight ratio of the precursor to CNTs. This simple and efficient approach may also be utilized to synthesize other high-purity materials using inorganic salt precursors in SC CO2-based solution.