Strapping plasmonic substrate with a reliable ability to anchor molecules and achieve reproducible result provides trustworthy opportunities for flourishing surface-enhanced Raman scattering (SERS) technique. Herein, a facile controllable in-situ anisotropic growth strategy was exploited to anchor gold nanowires (Au NWs) onto two-dimensional g-C3N4 nanosheets (g-C3N4/Au NWs), facilitating a sensitive and recyclable SERS sensor for gaseous analytes. Benefiting from the attractive enrichment effect of the brush-like surface formed by numerous small Au NWs as well as their rich nanotips-mediated enhancement capability, the hybrid substrate showed an outstanding performance in SERS-based detection of trace 4-Aminothiophenol (4-ATP) molecules, demonstrating a monitoring limitation down to 10−8 M even in atmosphere. Satisfyingly, under visible light illumination, the efficient green photocatalytic ability derived from the g-C3N4 supporting matrix rendered reusable capability for the substrate, whose SERS signal was kept at a persistent high level throughout 6 cycles. Attributed to the narrow line width of SERS spectrum, the 4-ATP assay under the interference of 2-naphthalenethiol (2-NAT) was acquired in gas phase and the dependable recovery rates from 85.4 to 93.9% were confirmed as well. Thanks to the intriguing features including excellent sensitivity and recyclability, the g-C3N4/Au NWs substrate proposed here will pave the way toward the potential application of SERS technique in multiplexed gaseous detection.