Carbon nanotubes (CNTs) with macroscopically ordered structures (e.g., aligned or patterned mats, fibers, and sheets) and associated large surface areas have proven promising as new CNT electroactive polymer materials (CNT-EAPs) for the development of advanced chemical and biological sensors. The functionalization of CNTs with many biological species to gain specific surface characteristics and to facilitate electron transfer to and from them for chemical- and bio-sensing applications is an area of intense research activity. Mechanical actuation generated by CNT-EAPs is another exciting electroactive function provided by these versatile materials. Controlled mechanical deformation for actuation has been demonstrated in CNT mats, fibers, sheets, and individual nanotubes. This article summarizes the current status and technological challenges for the development of electrochemical sensors and electromechanical actuators based on carbon nanotube electroactive materials.