With the prosperous development of artificial intelligence, medical diagnosis and electronic skins, wearable electronic devices have drawn much attention in our daily life. Flexible pressure sensors based on carbon materials with ultrahigh sensitivity, especially in a large pressure range regime are highly required in wearable applications. In this work, graphene membrane with a layer-by-layer structure has been successfully fabricated via a facile self-assembly and air-drying (SAAD) method. In the SAAD process, air-drying the self-assembled graphene hydrogels contributes to the uniform and compact layer structure in the obtained membranes. Owing to the excellent mechanical and electrical properties of graphene, the pressure sensor constructed by several layers of membranes exhibits high sensitivity (52.36 kPa⁻¹) and repeatability (short response and recovery time) in the loading pressure range of 0–50 kPa. Compared with most reported graphene-related pressure sensors, our device shows better sensitivity and wider applied pressure range. What’s more, we demonstrate it shows desired results in wearable applications for pulse monitoring, breathing detection as well as different intense motion recording such as walk, run and squat. It’s hoped that the facilely prepared layer-by-layer graphene membrane-based pressure sensors will have more potential to be used for smart wearable devices in the future.

随着人工智能，医学诊断和电子皮肤的蓬勃发展，可穿戴电子设备在我们的日常生活中引起了很多关注。在可穿戴应用中，特别需要具有超高灵敏度的基于碳材料的柔性压力传感器，尤其是在大压力范围内。在这项工作中，通过简便的自组装和风干（SAAD）方法成功地制造了具有逐层结构的石墨烯膜。在SAAD方法中，将自组装的石墨烯水凝胶风干有助于获得的膜中均匀且致密的层结构。由于石墨烯的优异的机械和电性能，由多层膜构成的压力传感器具有很高的灵敏度（52.36 kPa ^-1）和在0–50 kPa的加载压力范围内的重复性（响应时间和恢复时间短）。与大多数报道的石墨烯相关压力传感器相比，我们的设备显示出更高的灵敏度和更宽的施加压力范围。此外，我们证明它在可穿戴应用中显示出理想的结果，可用于脉搏监测，呼吸检测以及各种剧烈运动记录（如步行，跑步和下蹲）。希望将来容易制备的基于层状石墨烯膜的压力传感器在智能穿戴设备中具有更大的潜力。