The theory of high entropy‐dissipative structure is confined to high‐entropy alloys and their oxide materials under harsh conditions, but it is very difficult to obtain high entropy‐dissipative structure for smart sensors based on polymers and metal oxides under mild conditions. Moreover, multiple signal coupling effect heavily hinder the sensor applications, and current multimodal integrated devices can solve two signal‐decoupling, but need very complicated process way. In this work, new synthesis concept is the first time to fabricate high entropy‐dissipative conductive layer of smart sensors with triple‐signal response and self‐decoupling ability within poly‐pyrrole/zinc oxide (PPy/ZnO) system. The sensor (SPZ20) amplifies pressure (17.54%/kPa) and gas (0.37%/ppm), reduces humidity (0.41%/% RH) and temperature (0.12%/°C) signals, simultaneously achieving the triple self‐decoupling effect of pressure and gas in the complex temperature‐humidity field because of the enlarged pressure‐contact area, enhanced gas‐responsive sites, altered vapor path and its own heat insulation function. Additionally, it inherits the strong robustness (500 rubbing, washing, and heating or freezing cycles) and endurance (10 000 photo‐purification cycles) of traditional high‐entropy materials for information transmission and smart alarms in emergencies or harsh environments. This work gives a new insight into the multiple‐signal response and smart flexible electronic design from natural fibers.