A hybrid system comprising bimetallic nanoparticles supported on carbon nanotubes (CNTs) was engineered to maximize the surface-enhanced Raman scattering signal from solution by generating a high density of hot spots with reproducible enhancing activity and long-term colloidal and optical stability. CNT@AgAu was employed as a bifunctional material to catalyze and monitor the controlled release of nitric oxide from aromatic nitrosothiols, as a function of the gold content.