Comprehensively understanding the interdependency between the orientated atomic array and intrinsic piezoelectricity in one-dimension (1D) tellurium (Te) crystals will greatly benefit their practical piezo-catalytic applications. Herein, we successfully synthesized the various 1D Te microneedles by precisely orientating the atomic growth orientation by tuning (100)/(110) planes ratios (Te-0.6, Te-0.3, Te-0.4) to reveal the secrets of piezoelectricity. Explicitly, the theoretical simulations and experimental results have solidly validated that the Te-0.6 microneedle grown along the [110] orientation possesses a stronger asymmetric distribution of Te atoms array causing the enhanced dipole moment and in-plane polarization, which boosts a higher transfer and separation efficiency of the electron and hole pairs and a higher piezoelectric potential under the same stress. Additionally, the orientated atomic array along the [110] has p antibonding states with a higher energy level, resulting in a higher CB potential and a broadened band gap. Meanwhile, it also has a much lower barrier toward the valid adsorption of H 2 O and O 2 molecules over other orientations, effectively conducive to the production of reactive oxygen species (ROS) for the efficient piezo-catalytic sterilization. Therefore, this study not only broadens the fundamental perspectives in understanding the intrinsic mechanism of piezoelectricity in 1D Te crystals but also provides a candidate 1D Te microneedle for practical piezo-catalytic applications.