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Graphene nanocomposites are a promising class of advanced materials for sensing applications; yet, their commercialization is hindered due to impurity incorporation during fabrication and high costs. The aim of this work is to prepare graphene–polysulfone (G−PSU) and graphene–polyvinylidene fluoride (G−PVDF) nanocomposites that perform as multifunctional sensors and are formed using a one-step, in situ exfoliation process whereby graphite is exfoliated into graphene nanoflakes (GNFs) directly within the polymer. This low-cost method creates a nanocomposite while avoiding impurity exposure since the raw materials used in the in situ shear exfoliation process are graphite and polymers. The morphology, structure, thermal properties, and flexural properties were determined for G−PSU and G−PVDF nanocomposites, as well as the electromechanical sensor capability during cyclic flexural loading, temperature sensor testing while heating and cooling, and electrochemical sensor capability to detect dopamine while sensing data wirelessly. G−PSU and G−PVDF nanocomposites show superior mechanical characteristics (gauge factor around 27 and significantly enhanced modulus), thermal characteristics (stability up to 500 °C and 170 °C for G−PSU and G−PVDF, respectively), electrical characteristics (0.1 S/m and 1 S/m conductivity for G−PSU and G−PVDF, respectively), and distinguished resonant peaks for wireless sensing (~212 MHz and ~429 MHz). These uniquely formed G−PMC nanocomposites are promising candidates as strain sensors for structural health monitoring, as temperature sensors for use in automobiles and aerospace applications, and as electrochemical sensors for health care and disease diagnostics.