Coagulation spinning produces structures such as fibers, ribbons, and yarns of carbon nanotubes. Stabilization, orientation, and shaping of spun materials are achieved by post-spinning processes. Advantages include the elimination of core-sheath effects due to carbonaceous contaminants, increasing mechanical properties, and eliminating dimensional instabilities in liquid electrolytes that previously prohibited the application of these spun materials in electrochemical devices. These advances enable the application of coagulation-spun carbon nanotube fibers, ribbons, and yarns in actuators, supercapacitors, and in devices for electrical energy harvesting.