Tea polyphenols, widely available and easily accessible in nature, readily complex with metal ions to form metal-phenolic networks. In this study, the mechanical properties of nanocellulose (CNF) aerogel were enhanced through directional freezing with tea polyphenol (TP). Subsequently, high-temperature pyrolysis was used to prepare tea polyphenol/iron-modified nanocellulose carbon aerogel(CTP/Fe@CNF), which exhibits excellent elasticity and sensing properties. When subjected to 80% deformation, the aerogel rapidly returns to its original height upon release of the external force, with its maximal stress decreasing by only about 6.2% after 400 compression cycles. It maintains a stable relative resistance change over prolonged compression and, when fixed to moving parts of the human body, such as finger joints, responds quickly and stably to motion changes. These characteristics highlight its potential as a flexible pressure sensor.