Microfiber devices are able to extend the micro/nano functionalities of materials or devices to the macroscopic scale with excellent flexibility and weavability, promising a variety of unique applications and, sometimes, also improved performance as compared with bulk counterparts. The fiber electrodes in these devices are often made of carbon materials (e.g. carbon nanotubes and graphene) because of their exceptional electrical, mechanical, and structural properties. Covering the latest developments and aiming to stimulate more exciting applications, we comprehensively review the preparation and applications of carbon-microfiber devices on energy conversion and storage, electronics, sensors and actuators.