The outstanding potential of microwave resonator-based energy-efficient gas sensors has been overshadowed by their underperforming gas sensing capabilities, especially insignificant sensitivity to detect low-concentration volatile organic compounds (VOCs). This unmet challenge persists primarily due to predominant metallic resonator structures, which further limit their wearable applications and pose environmental concerns. This work presents a laser-induced graphene (LIG)-enabled split-ring resonator (SRR) sensor on a flexible polyimide substrate for the rapid and sensitive detection of gaseous VOCs. To implement the sensor, the conductive traces of the SRR were created using a computer-controlled CO2 laser at an optimized power level, thus inducing 48 µm thick, conductive (24 S/cm) graphene layers on a polyimide substrate. The SRR gas sensor, in which LIG with three-dimensional networks of porosity serves as conductive and even gas-sensitive traces, benefits from a significantly enhanced interaction between the SRR’s electromagnetic field and VOC gases. As a proof of concept, a prototype of the LIG-enabled SRR was implemented and mounted on a test fixture. The developed gas sensor operated at a resonant frequency of 1.402 GHz, which exhibited rapid (∼17 s) and noticeable shifts when exposed to 200 ppm of different VOCs (acetone, ethanol, methanol, toluene, and isopropyl alcohol). Additionally, the sensor demonstrated a linear correlation between the resonant frequency and acetone gas concentration (1 ppm-200 ppm), with a sensitivity of 188 KHz/ppm. These electromagnetic and gas sensing results suggest that polyimide-derived LIG traces can replace metal microstrip lines in the SRR structure, opening up possibilities for high-performance microwave resonator gas sensors, even suitable for flexible and wearable applications.