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.