Flexible pressure sensors possess vast potential for various applications such as new energy batteries, aerospace engines, and rescue robots owing to their exceptional flexibility and adaptability. However, the existing sensors face significant challenges in maintaining long-term reliability and environmental resilience when operating in harsh environments with variable temperatures and high pressures (∼MPa), mainly due to possible mechanical mismatch and structural instability. Here, we propose a composite scheme for a flexible piezoresistive pressure sensor to improve its robustness by utilizing material design of near-zero temperature coefficient of resistance (TCR), radial gradient pressure-dividing microstructure, and flexible interface bonding process. The sensing layer comprising multiwalled carbon nanotubes (MWCNTs), graphite (GP), and thermoplastic polyurethane (TPU) was optimized to achieve a near-zero temperature coefficient of resistance over a temperature range of 25−70 °C, while the radial gradient microstructure layout based on pressure division increases the range of pressure up to 2 MPa. Furthermore, a flexible interface bonding process introduces a self-soluble transition layer by direct-writing TPU bonding solution at the bonding interface, which enables the sensor to achieve signal fluctuations as low as 0.6% and a high interface strength of up to 1200 kPa. Moreover, it has been further validated for its capability of monitoring the physiological signals of athletes as well as the long-term reliable environmental resilience of the expansion pressure of the power cell. This work demonstrates that the proposed scheme sheds new light on the design of robust pressure sensors for harsh environments.