Organic polymer-based composite materials with favorable mechanical performance and functionalities are keystones to various modern industries; however, the environmental pollution stemming from their processing poses a great challenge. In this study, by finding an autonomous phase separating ability of fungal mycelium, a new material fabrication approach is introduced that leverages such biological metabolism-driven, mycelial growth-induced phase separation to bypass high-energy cost and labor-intensive synthetic methods. The resulting self-regenerative composites, featuring an entangled network structure of mycelium and assembled organic polymers, exhibit remarkable self-healing properties, being capable of reversing complete separation and restoring ≈90% of the original strength. These composites further show exceptional mechanical strength, with a high specific strength of 8.15 MPa g.cm⁻³, and low water absorption properties (≈33% after 15 days of immersion). This approach spearheads the development of state-of-the-art living composites, which directly utilize bioactive materials to “self-grow” into materials endowed with exceptional mechanical and functional properties.

A flexible sensor with excellent pressure, temperature, and bending sensitivity is fabricated based on the conductive skeleton material with hierarchical porous structure. The conductive skeleton material is composed of carbon fibres (CFs) and multiwalled carbon nanotubes (MWCNTs), in which lay perpendicular to each other CFs are used as conductive frames, while MWCNTs are served as bridges to connect the CFs and increase the conductive network formation. Owing to the unique structure and the conductive materials, the as-prepared sensor exhibits a high-pressure sensing performance of 42.7 kPa (0–1 kPa), fast response, relaxation times of<100 ms, wide working range of 0–60 kPa, and high stability over more than 6000 cycles. Furthermore, the fabricated sensor presents a high thermal sensitivity of 2.46 °C⁻¹ between 30 and 40 °C, excellent bending sensitivity of 95.5 % rad⁻¹ in the working range of 0–180°, and great flexibility (over 1000 cycles), demonstrating its potential applications in multifunctional wearable electronics.