随着社会发展，人们对可检测健康与运动信息的柔性可穿戴设备的需求日益提高。因此，柔性可穿戴器件的研究备受关注，各类柔性器件被开发出来，例如，应力/应变传感器、电生理信号传感器、电化学传感器等。柔性材料是构建柔性器件的基础，相关研究是该领域发展的基础。石墨烯作为一种新型纳米碳材料，具有良好的机械和化学稳定性、柔性、导电性以及结构和性能可调等优点，是一种很有潜力的柔性材料。本论文针对柔性可穿戴器件的应用需求，开展石墨烯的结构设计和可控制备技术研究，开发石墨烯的便捷表征和转移技术，并进行功能复合，成功制备了石墨烯基高灵敏压力传感器、图像传感器等柔性器件。主要创新性成果如下：一、实现了多种特殊形貌石墨烯的可控生长。通过对基底的处理和生长参数的调控，实现了大尺寸六边形石墨烯晶畴、取向一致的五边形石墨烯晶畴、具有指纹结构的石墨烯薄膜、以及以天然蚕丝作为固态碳源而生长的氮掺杂石墨烯等多种石墨烯材料的可控生长，研究了其生长机理和基本性质，为后续研究奠定了基础。二、发展了水蒸气辅助法，实现了石墨烯无损、可控的光学表征。基于基底上石墨烯的润湿行为，设计了水蒸气辅助方法，实现了多种基底表面的石墨烯无损、可控的光学可视化表征。该方法操作简单、无污染、可重复，为石墨烯及其他二维材料的研究提供了一种便捷的表征方法。三、发明了一种可移除石墨烯“保鲜膜”。基于石墨烯良好的化学稳定性和阻气性，以热释放胶带为辅助，通过大面积石墨烯薄膜的生长和转移，设计制备了可用于保护空气中不稳定二维材料的石墨烯“保鲜膜”。该“保鲜膜”操作简单、保护效果好、并可通过热释放胶带移除，为空气中不稳定二维材料的研究提供了新技术。四、设计制备了指纹状石墨烯基高性能柔性压力传感器。利用化学气相沉积获得的指纹状石墨烯薄膜和印模天然植物叶片得到的具有多级结构的柔性基底，构筑了具有高灵敏度、宽工作范围的柔性压力传感器，分析了压力传感器的结构-性能依赖关系，并展示了其在微小物体检测、人体健康监测和发声康复训练中的应用。五、设计制备了钙钛矿/石墨烯异质结基柔性图像传感器。基于石墨烯可诱导二维材料横向生长的性质，以单层石墨烯薄膜为生长模板，利用化学气相沉积法制备了高质量的有机-无机杂化钙钛矿/石墨烯异质结。以此异质结作为光吸收层构筑了柔性光电探测器和具有24×24像素的柔性类视网膜图像传感器，并展示了其在视觉成像中的应用。

With the development of society, the demand for flexible wearable devices that can detect health and sports information is increasing. Therefore, research on flexible wearable devices has attracted much attention, and various types of flexible devices have been developed, such as stress/strain sensors, electrophysiological signal sensors, and electrochemical sensors. Flexible materials are the basis for building flexible devices, and related research is the foundation of development in this field. Graphene, as a new type of nano-carbon material, has good mechanical and chemical stability, flexibility, electrical conductivity, and adjustable structure and performance. It is a very flexible material with great potential. In this paper, we focus on the application of flexible wearable electronic devices. By designing and controlling the structure of graphene materials, developing characterization and transfer technologies, and implementing functional compounding, we explore the application of graphene materials in flexible wearable devices. The main research results are as follows:1. Controllable growth of graphene with a variety of special morphologies. Through the treatment of the substrate and the adjustment of the growth parameters, large-sized hexagonal graphene crystal domains, uniformly oriented pentagonal graphene crystal domains, graphene films with fingerprint structures have been prepared. Furtherly, high-quality nitrogen-doped graphene with different morphologies have been realized using natural silk as a nitrogen-containing solid carbon source. The growth mechanism and basic properties have been studied, laying a foundation for subsequent research.2.Develop non-destructive, controllable graphene optical characterization technology. Based on the water wetting behavior of graphene on the substrate, a water vapor assisted method was designed to realize non-destructive optical visualization of graphene on various substrate surfaces. The method is simple, non-polluting, and repeatable, and provides a convenient method for characterizing graphene and other two-dimensional materials.3.Design a removable graphene "seal wrap". Based on the excellent stability and gas barrier properties of graphene, a graphene "seal wrap" was prepared through the growth and transfer of a large area of intact graphene film and assisted by a heat release tape, which can be used to protect air unstable two-dimensional material. The graphene "seal wrap" has simple operation, good protection effect, and can be removed through heat release tape, which provides ideas for the research and application of unstable two-dimensional materials in the air.4.Construct high-performance flexible pressure sensor based on fingerprint-like graphene film. According to the above-mentioned design, preparation, characterization and transfer of graphene, we analyzed the influencing factors of flexible pressure sensors to prepare a fingerprint-like three-dimensional graphene film and a flexible PDMS substrate with multi-level microstructure. Furtherly, we constructed a flexible pressure sensor with high sensitivity and wide working range, and demonstrated its application in the detection of small objects, human health monitoring, and vocal rehabilitation training.5.Construct high-performance flexible image sensor based on MAPbI3/graphene heterojunction. By analyzing the limiting factors of traditional organic-inorganic hybrid perovskites in photovoltaic devices, we used graphene as a template to synthesize MAPbI3/graphene heterostructure based on the excellent photoelectric properties and the properties that can induce the lateral growth of two-dimensional materials of graphene. We used the heterojunction as a light absorbing layer to construct a flexible photodetector and a flexible photodetector array with 24 × 24 pixels as image sensors, showing their applications in visual imaging.