In this work, a room-temperature atmospheric pressure direct-current plasma has been deployed for the one-step synthesis of gold nanoparticle/carboxyl group-functionalized carbon nanotube (AuNP/CNT-COOH) nanohybrids in aqueous solution for the first time. Uniformly distributed AuNPs are formed on the surface of CNT-COOH, without the use of reducing agents or surfactants. The size of the AuNP can be tuned by changing the gold salt precursor concentration. UV–vis, ζ-potential, and X-ray photoelectron spectroscopy suggest that carboxyl surface functional groups on CNTs served as nucleation and growth sites for AuNPs and the multiple potential reaction pathways induced by the plasma chemistry have been elucidated in detail. The nanohybrids exhibit significantly enhanced Raman scattering and photothermal conversion efficiency that are essential for potential multimodal cancer treatment applications.