Carbon nanotubes (CNTs) are nanoscale tubular materials with superior mechanical strength and electronic properties. However, the conventional CNTs are inherently non‐piezoelectric, mainly due to the lack of polar structures with pure carbon elements. The direct synthesis of fully conjugated and polarized organic nanotubes with desired piezoelectric properties remains a challenge. Herein, we report the bottom‐up synthesis of a new type of covalent triazine‐based nanotube (CTN‐1) as a novel piezoelectric material. The CTN‐1 comprises of high surface area, nitrogen‐rich and fully conjugated structure, which provides a series of merits for piezoelectric catalytic processes. These structural features combined with one‐dimensional tubular morphology endow CTN‐1 with excellent mechanical stimuli response and thus displaying prominent piezoelectric properties via pronounced nanocurvature effect. We further show that the CTN‐1 enables the efficient synthesis of H2O2 from water in the air via mechanical energy conversion, with an excellent piezocatalytic H2O2 evolution rate of 4115 μmol g‐1 h‐1, which exceeds all other reported piezoelectric materials. The piezocatalysis by the CTN‐1 can be practically integrated into a self‐Fenton system, which exhibits excellent pollutant degradation capability. This work demonstrates the enormous potential of a new type of piezoelectric synthetic nanotube from organic frameworks for the in‐situ synthesis valuable chemicals.