Integrating real‐time electrical gas sensing and highly identifiable surface‐enhanced Raman spectroscopy (SERS) for volatile organic compounds (VOCs) monitoring holds significant potential for safeguarding public health and safety. However, this technique remains in the proof‐of‐concept stage because the performance and reproducibility of devices fall short of meeting the practical application requirements. This work addresses this challenge by employing vortex engineering on a bifunctional dual‐layer array of Ni‐doped SnO2 (Ni‐SnO2) bowl‐coated on Ni‐SnO2/Au/SiO2 and developing highly reproducible device fabrication. In the dual‐layer array, vortices generated in upper Ni‐SnO2 bowls slow down the VOC flow and direct its delivery to gaps between lower Ni‐SnO2/Au/SiO2 units that are critical to SERS and electrical sensing. Experimental results show that the vortex effect in the array enables a low limit of detection of 10 ppb with a response and recovery in seconds. The excellent practicality of the array has been demonstrated through a ca. 100 hours of quantitative dual‐monitoring of styrene in a spacious environment (~60 m3) with a 5‐meter distance between the leakage source and the array. This work advances dual‐monitoring sensors for practical applications and offers insights for designing gas‐sensing materials and devices.