Sensitivity is a crucial parameter for flexible pressure sensors and electronic skins. While introducing microstructures (e.g., micro-pyramids) can effectively improve the sensitivity, it in turn leads to a limited pressure-response range due to the poor structural compressibility. Here, we report a strategy of engineering intrafillable microstructures that can significantly boost the sensitivity while simultaneously broadening the pressure responding range. Such intrafillable microstructures feature undercuts and grooves that accommodate deformed surface microstructures, effectively enhancing the structural compressibility and the pressure-response range. The intrafillable iontronic sensor exhibits an unprecedentedly high sensitivity (Smin > 220 kPa−1) over a broad pressure regime (0.08 Pa-360 kPa), and an ultrahigh pressure resolution (18 Pa or 0.0056%) over the full pressure range, together with remarkable mechanical stability. The intrafillable structure is a general design expected to be applied to other types of sensors to achieve a broader pressure-response range and a higher sensitivity.

Flexible electronic skins (e-skins) with high sensitivity and broad-range pressure sensing are highly desired in artificial intelligence, and humanmachine interaction. Capacitive-type e-skins have a simple configuration, but the change in dimensions of the dielectric layer is often quite limited, although introducing surface microstructures might improve the sensitivity in some extent. Moreover, such surface structures typically require costly microfabrication methods to fabricate. Here, a low-cost microstructured ionic gel (MIG) with uniform cone-like surface microstructures for highperformance capacitive e-skins is reported. The MIG film is templated from a Calathea zebrine leaf using soft lithography, and sandwiched by two flexible electrodes. The device exhibits a low limit of detection down to 0.1 Pa, a ultrahigh sensitivity of 54.31 kPa −1 in the low pressure regime (<0.5 kPa), and the sensitivity keeps larger than 1 kPa −1 over a broad-range pressure from 0.1 Pa to 115 kPa. Electric double layers (EDL) form on both the top and bottom interfaces, and the area of EDL of the rough interface increases as the cones are compressed. Such ionic skins with biomimetic gel templated Calathea zebrine leaf allow for sensitive tactile sensing in the applications of human-machine interaction.

Electronic skins (e-skins) are devices that can respond to mechanical stimuli and enable robots to perceive their surroundings. A great challenge for existing e-skins is that they may easily fail under extreme mechanical conditions due to their multilayered architecture with mechanical mismatch and weak adhesion between the interlayers. Here we report a flexible pressure sensor with tough interfaces enabled by two strategies: quasi-homogeneous composition that ensures mechanical match of interlayers, and interlinked microconed interface that results in a high interfacial toughness of 390 J·m−2. The tough interface endows the sensor with exceptional signal stability determined by performing 100,000 cycles of rubbing, and fixing the sensor on a car tread and driving 2.6 km on an asphalt road. The topological interlinks can be further extended to soft robot-sensor integration, enabling a seamless interface between the sensor and robot for highly stable sensing performance during manipulation tasks under complicated mechanical conditions.

Flexible pressure sensors that have high sensitivity, high linearity, and a wide pressure-response range are highly desired in applications of robotic sensation and human health monitoring. The challenge comes from the incompressibility of soft materials and the stiffening of microstructures in the device interfaces that lead to gradually saturated response. Therefore, the signal is nonlinear and pressure-response range is limited. Here, we show an iontronic flexible pressure sensor that can achieve high sensitivity (49.1 kPa–1), linear response (R 2 > 0.995) over a broad pressure range (up to 485 kPa) enabled by graded interlocks of an array of hemispheres with fine pillars in the ionic layer. The high linearity comes from the fact that the pillar deformation can compensate for the effect of structural stiffening. The response-relaxation time of the sensor is <5 ms, allowing the device to detect vibration signals with frequencies up to 200 Hz. Our sensor has been used to recognize objects with different weights based on machine learning during the gripper grasping tasks. This work provides a strategy to make flexible pressure sensors that have combined performances of high sensitivity, high linearity, and wide pressure-response range.