The bioinspired microdevices have made significant strides in various applications including human motion and health detection. However, the facile and highly efficient fabrication approach of flexible pressure sensors remains a great challenge. Herein, inspired by the gecko's foot structure, a flexible pressure sensor with microdomes structures was one‐step fabricated by tip‐assisted on‐demand electrohydrodynamic jet (EHD‐jet) printing method. Ascribed to the interlocking electrodes with microdome structure substantially enlarged 3D deformation rates. When the microdromes structure is under pressure, the resistivity of the CNTs film coated on the surface of the microdomes structure will change remarkably. By using the combined effect of assisted tip and ring focusing electrode, the influence and constraints on microstructure fabrication caused by substrate material and morphology are minimized. The desired uniform structures can be adjusted rapidly by changing the printing parameters and liquid properties. The high length‐height ratio (0.64) of microdomes, notably enhances the sensitivity, the minimum detection limit is 2 Pa and the response time is 40 ms. Finally, the bionic flexible sensor shows excellent performance in capable of detecting pressure, sound vibrations, and human motion. This work introduces a previously unexplored method for the high‐efficiency fabrication of micro‐nano patterns for bionic flexible sensors, with potential applications in wearable devices and human health detection.This article is protected by copyright. All rights reserved