There has been enormous interest in technologies that generate electricity from ambient energy such as solar, thermal, and mechanical energy, due to their potential for providing sustainable solutions to the energy crisis. One driving force behind the search for new energy-harvesting technologies is the desire to power sensor networks and portable devices without batteries, such as self-powered wearable electronics, human health monitoring systems, and implantable wireless sensors. Various energy harvesting technologies have been demonstrated in recent years. Among them, electrochemical, hydroelectric, triboelectric, piezoelectric, and thermoelectric nanogenerators have been extensively studied because of their special physical properties, ease of application, and sometimes high obtainable efficiency. Multifunctional carbon nanotubes (CNTs) have attracted much interest in energy harvesting because of their exceptionally high gravimetric power outputs and recently obtained high energy conversion efficiencies. Further development of this field, however, still requires an in-depth understanding of harvesting mechanisms and boosting of the electrical outputs for wider applications. Here, various CNT-based energy harvesting technologies are comprehensively reviewed, focusing on working principles, typical examples, and future improvements. The last section discusses the existing challenges and future directions of CNT-based energy harvesters.