<p>The potential of iontronic capacitive pressure sensors (ICPSs) in wearable technology applications is fundamentally constrained by an inherent trade-off between sensitivity and detection range. To overcome this limitation, we propose a novel strategy termed ‘micro-electric double layer (micro-EDL) engineering’. This approach is achieved through the chemical design of a nanocomposite dielectric, in which multi-walled carbon nanotubes (MWCNTs) form a percolated network, thereby generating a dense array of pressure-responsive nano-capacitors. When synergistically integrated with a hierarchical MoS₂/NiCo-LDH electrode that offers abundant pseudocapacitive interfaces, the resulting sensor demonstrates a combination of performance metrics: an ultrahigh sensitivity of 67,095 kPa⁻¹ at 1 kHz across a broad detection range of up to 1.3 MPa, response and recovery times of 4 and 5 ms, respectively, and outstanding durability exceeding 18,000 cycles. Practical validation revealed a classification accuracy of 100% in recognizing complex gestures and gait patterns, highlighting the device’s applicability in real-world scenarios. These findings highlight micro-EDL engineering as a promising approach for enhancing next-generation iontronic devices, offering valuable insights into their electrochemical mechanisms.</p>