Macroscopic ribbon-like assemblies of carbon nanotubes (CNTs) are functionalised using a simple direct-current-based plasma–liquid system, with oxygen and nitrogen functional groups being added. These modifications have been shown to reduce the contact angle of the ribbons, with the greatest reduction being from 84° to 35°. The ability to improve the wettability of the CNTs is of paramount importance for producing nanofluids, with relevance for a number of applications. Here, in particular, we investigate the efficacy of these samples as nanofluid additives for solar–thermal harvesting. Surface treatments by plasma-induced non-equilibrium electrochemistry are shown to enhance the stability of the nanofluids, allowing for full redispersion under simulated operating conditions. Furthermore, the enhanced dispersibility results in both a larger absorption coefficient and an improved thermal profile under solar simulation.