Abstract Recently, conductive metal−organic frameworks (MOFs) as the active material have provided broad prospects for electronic device application. The positioning technologies for MOFs enable the fabrication of novel microstructures, which can modulate the morphology of the material and tune the properties for the targeted application. Herein, a template‐method is used to synthesize the hierarchical structure of MOF hybrid array (MHA) on copper mesh (MHA@Mesh) for flexible sensor. Finite element method (FEM) results indicate that the 3D hierarchical MHA@Mesh can mimic the micro/nanoscale structure of human skin, which enables an interlocking contact. MHA@Mesh‐based flexible sensor presents rapid response rate (<1 ms) and high sensitivity (up to 307 kPa −1 ) which is 20 times higher than that of MHA@Foil‐based sensor (15 kPa −1 ). The flexible pressure device could be applied to monitor the finger motion and human pulses. Moreover, the music recognition can be performed by integrating the MOFs hardware sensors with machine learning algorithms. Overall, this design concept of 3D hierarchical microarray structures demonstrates potential in the fields of wearable technologies and human–machine interfaces.