High‐sensitivity flexible wireless passive sensors with multiple parameters sensing capability are highly demanded for industrial production, structural health monitoring, and medical care. In this study, a microstructure‐enhanced temperature and pressure dual‐mode inductance capacitance (LC) sensor is developed with a particle swarm optimization‐back propagation (PSO‐BP) algorithm for simultaneous measurement of temperature and pressure. In the device, two interdigital electrodes connected at different parts of an inductor is used to realize dual‐mode measurement of pressure and temperature, with reduced volume and cost of the device as well as avoided interaction of the superimposed inductance. The sandpaper‐molded polydimethylsiloxane microstructures are employed to enhance the device sensitivity, with six and three times of improvement in temperature and pressure sensitivity, respectively. A PSO‐BP neural network suitable for regression analysis of low dimensional small sample data is constructed to achieve the simultaneous measurement of pressure and temperature with an accuracy up to 94%. Furthermore, investigations have proved the promising applications of the dual‐mode LC sensor in health monitoring of lithium‐ion batteries and detection of plantar pressure for medical care.