Graphene aerogels hold huge promise for the development of high-performance pressure sensors for future human-machine interfaces due to their ordered microstructure and conductive network. However, their application is hindered by the limited strain sensing range caused by the intrinsic stiffness of the porous microstructure. Herein, an anisotropic cross-linked chitosan and reduced graphene oxide (CCS-rGO) aerogel metamaterial is realized by reconfiguring the microstructure from a honeycomb to a buckling structure at the dedicated cross-section plane. The reconfigured CCS-rGO aerogel shows directional hyperelasticity with extraordinary durability (no obvious structural damage after 20 000 cycles at a directional compressive strain of ≤0.7). The CCS-rGO aerogel pressure sensor exhibits an ultrahigh sensitivity of 121.45 kPa-1, an unprecedented sensing range, and robust mechanical and electrical performance. The aerogel sensors are demonstrated to monitor human motions, control robotic hands, and even integrate into a flexible keyboard to play music, which opens a wide application potential in future human-machine interfaces.