The availability of robust, versatile, and efficient photocatalysts is the main bottleneck in practical applications of photocatalytic degradation of organic pollutants. Herein, N‐WO3/Ce2S3 nanotube bundles (NBs) are synthesized and successfully immobilized on a carbon textile, resulting in a flexible and conducting photocatalyst. Due to the large interfacial area between N‐WO3 and Ce2S3, the interwoven 3D carbon architecture and, more importantly, the establishment of a heterojunction between N‐WO3 and Ce2S3, the resultant photocatalyst exhibits excellent light absorption capacity and superior ability to separate photoinduced electron–hole pairs for the photocatalytic degradation of organic compounds in air and water media. Theoretical calculations confirm that the strong electronic interaction between N‐WO3 and Ce2S3 can be beneficial to the enhancement of the charge carrier transfer dynamics of the as‐prepared photocatalyst. This work provides a new protocol for constructing efficient flexible photocatalysts for application in environmental remediation.