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Here an all-purpose fibrous electrode based on MoS2 is demonstrated, which can be employed for versatile energy harvesting and storage applications. In this coaxial electrode, ultrathin MoS2 nanofilms are grown on TiO2 nanoparticles coated carbon fiber. The high electrochemical activity of MoS2 and good conductivity of carbon fiber synergistically lead to the remarkable performances of this novel composite electrode in fibrous dye-sensitized solar cells (showing a record-breaking conversion efficiency of 9.5%) and high-capacity fibrous supercapacitors. Furthermore, a self-powering energy fiber is fabricated by combining a fibrous dye-sensitized solar cell and a fibrous supercapacitor into a single device, showing very fast charging capability (charging in 7 s under AM1.5G solar illumination) and an overall photochemical-electricity energy conversion efficiency as high as 1.8%. In addition, this wire-shaped electrode can also be used for fibrous Li-ion batteries and electrocatalytic hydrogen evolution reactions. These applications indicate that the MoS2-based all-purpose fibrous electrode has great potential for the construction of high-performance flexible and wearable energy devices.