The surging growth of the pharmaceutical industry is a result of the rapidly increasing human population, which has inevitably led to new biomedical and environmental issues. Aside from the quality control of pharmaceutical production and drug delivery, there is an urgent need for precise, sensitive, portable, and cost-effective technologies to track patient overdosing and to monitor ambient water sources and wastewater for pharmaceutical pollutants. The development of advanced nanomaterial-based electrochemical sensors and biosensors for the detection of pharmaceutical compounds has garnered immense attention due to their advantages, such as high sensitivity and selectivity, real-time monitoring, and ease of use. This review article surveys state-of-the-art nanomaterials-based electrochemical sensors and biosensors for the detection and quantification of six classes of significant pharmaceutical compounds, including anti-inflammatory, anti-depressant, anti-bacterial, anti-viral, anti-fungal, and anti-cancer drugs. Important factors such as sensor/analyte interactions, design rationale, fabrication, characterization, sensitivity, and selectivity are discussed. Strategies for the development of high-performance electrochemical sensors and biosensors tailored toward specific pharmaceuticals are highlighted to provide readers and scientists with an extensive toolbox for the detection of a wide range of pharmaceuticals. Our aims are two-fold: (i) to inspire readers by further elucidating the properties and functionalities of existing nanomaterials for the detection of pharmaceuticals; and (ii) to provide examples of the potential opportunities that these devices have for the advanced sensing of pharmaceutical compounds toward safeguarding human health and ecosystems on a global scale.