AbstractThe tactile pressure sensor is of great significance in flexible electronics, but sensitivity customization over the required working range with high linearity still remains a critical challenge. Despite numerous efforts to achieve high sensitivity and a wide working range, most sensitive microstructures tend to be obtained only by inverting naturally existing templates without rational design based on fundamental contact principles or models for piezoresistive pressure sensors. Here, a positive design strategy with a hyperelastic model and a Hertzian contact model for comparison was proposed to develop a flexible pressure sensor with highly customizable linear sensitivity and linearity, in which the microstructure distribution was precalculated according to the desired requirement prior to fabrication. As a proof of concept, three flexible pressure sensors exhibited sensitivities of 0.7, 1.0, and 1.3 kPa⁻¹ over a linear region of up to 200 kPa, with a low sensitivity error (<5%) and high linearity (~0.99), as expected. Based on the superior electromechanical performance of these sensors, potential applications in physiological signal recognition are demonstrated as well, and such a strategy could shed more light on demand-oriented scenarios, including designable working ranges and linear sensitivity for next-generation wearable devices.