conductivity, [17][18][19][20] and the design of new structures for the material. [21][22][23][24] MXene (Ti 3 C 2 T x ), an emerging 2D nanomaterial composed of transition metal carbide/nitride, has excellent electrical conductivity due to its inherent ease of building conductive networks and shows significant application potentials in the field of smart sensors in recent years. [25][26][27] For example, Kedambaimoole et al. used a laser cutting method to prepare MXene thin films for skin conformable tattoo sensors with high strain sensitivity, which corresponds to the sensing mechanism of nano-crack generation and propagation. [28] Besides, Pu et al. proposed a feasible strain sensor fabrication strategy based on strain localization-induced fracture mechanism to achieve highly sensitive signal output at small strain by the change of fracture crack inside the material under stress. [29] In general, MXene-based flexible electronic devices are often unable to maintain good signal output stability while simultaneously realizing high sensitivity and wide detection range. Rational macrostructure design of MXene film has been proved to be an effective method to realize the above goal. Unfortunately, regardless of many structures being applied to construct MXene-based flexible sensitive sensors in the past years, defects in the structure itself may also lead to a short working lifetime and unstable signal output. Accordingly, in consideration of the demands in practical applications, suitable surface structure design to construct high-performance MXene-based flexible sensitive sensors is of great importance.In view of the above content, we in the present work develop a simple and low-cost substrate shrinkage method to prepare flexible pyramid-like MXene film (PMF) and further assemble it into high-quality flexible and wearable pressure sensor (PMFS). Delightedly, the unique micro-pyramidal microstructure endows the sensor with high sensitivity (64.56 kPa −1 ) and wide sensing range (4.9 Pa-98 kPa). More importantly, benefiting from the good stability characteristics of the angular cone structure, [30][31][32] the prepared pressure sensor could output stable signal output and exhibit long-time service life (18 000 cycles). Based on the remarkable sensing characteristics, the resulting pressure sensor was further applied to real-time detection of human physiological signals and recognition of facial subtle expressions, demonstrating its broad application prospect in future flexible intelligent wearable electronic devices.