This article reviews applications of nanoscale carbon-based materials in heavy metal sensing and detection. These materials, including single-walled carbon nanotubes, multi-walled carbon nanotubes and carbon nanofibers among others, have unique and tunable properties enabling applications in various fields spanning from health, electronics and the environment sector. Specifically, we highlight the unique properties of these materials that enable their applications in the sorption and preconcentration of heavy metals ions prior to detection by spectroscopic, chromatographic and electrochemical techniques. We also discuss their distinct properties that enable them to be used as novel electrode materials in sensing and detection. The fabrication and modification of these electrodes is discussed in detail and their applications in various electrochemical techniques such as voltammetric stripping analysis, potentiometric stripping analysis, field effect transistor-based devices and electrical impedance are critically reviewed. Perspectives and futures trends in the use of these materials in heavy metal sensing and detection will also be highlighted.