Novel in-situ freeze polymerization assisted layer-by-layer self-assembly method was utilized to prepare robust regenerated cellulose fiber-polypyrrole (RCF-PPy) composite fibers with high-conductivity, where transverse-longitudinal polypyrrole growth on RCF was regulated by using Lewis acid FeCl3 in crystalline ice state with the template etching and oxidation effects. The RCF-PPy3 exhibited high strength (1.01 cN/dtex) and exceptional durability, withstanding mechanical deformation, friction (100 cycles), and ultrasonic washing (50 times), addressing the issues of poor interface adhesion and conductivity stability of conductive fibers. Furthermore, the composite fiber demonstrated high electrical conductivity of 87.66 mS cm−1 and outstanding sensing performances for monitoring strain, pressure, temperature (0.34 %/°C), and humidity (0.895 %/RH). Based on RCF-PPy3, a pressure sensor was constructed as a human–machine interface electronic device, achieving sedentary reminders, fingertip information transmission, indicating great potential applications in intelligent wearable fiber electronic devices.