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The interaction of carbon-based nanomaterials and ionic liquids (ILs) has been thoroughly exploited for diverse electroanalytical solutions since the first report in 2003. This combination, either through covalent or non-covalent functionalization, takes advantage of the unique characteristics inherent to each material, resulting in synergistic effects that are conferred to the electrochemical (bio)sensing system. From one side, carbon nanomaterials offer miniaturization capacity with enhanced electron transfer rates at a reduced cost, whereas from the other side, ILs contribute as ecological dispersing media for the nanostructures, improving conductivity and biocompatibility. The present review focuses on the use of this interesting type of nanocomposites for the development of (bio)sensors specifically for pharmaceutical detection, with emphasis on the analytical (bio)sensing features. The literature search displayed the conjugation of more than 20 different ILs and several carbon nanomaterials (MWCNT, SWCNT, graphene, carbon nanofibers, fullerene, and carbon quantum dots, among others) that were applied for a large set (about 60) of pharmaceutical compounds. This great variability causes a straightforward comparison between sensors to be a challenging task. Undoubtedly, electrochemical sensors based on the conjugation of carbon nanomaterials with ILs can potentially be established as sustainable analytical tools and viable alternatives to more traditional methods, especially concerning in situ environmental analysis.

Pharmaceuticals, as a contaminant of emergent concern, are being released uncontrollably into the environment potentially causing hazardous effects to aquatic ecosystems and consequently to human health. In the absence of well-established monitoring programs, one can only imagine the full extent of this problem and so there is an urgent need for the development of extremely sensitive, portable, and low-cost devices to perform analysis. Carbon-based nanomaterials are the most used nanostructures in (bio)sensors construction attributed to their facile and well-characterized production methods, commercial availability, reduced cost, high chemical stability, and low toxicity. However, most importantly, their relatively good conductivity enabling appropriate electron transfer rates—as well as their high surface area yielding attachment and extraordinary loading capacity for biomolecules—have been relevant and desirable features, justifying the key role that they have been playing, and will continue to play, in electrochemical (bio)sensor development. The present review outlines the contribution of carbon nanomaterials (carbon nanotubes, graphene, fullerene, carbon nanofibers, carbon black, carbon nanopowder, biochar nanoparticles, and graphite oxide), used alone or combined with other (nano)materials, to the field of environmental (bio)sensing, and more specifically, to pharmaceutical pollutants analysis in waters and aquatic species. The main trends of this field of research are also addressed.