Noble metal nanoparticles (NMNPs) assembly substrates with strongly enhanced local electromagnetic fields provide new possibilities for surface-enhanced Raman spectroscopy (SERS) sensing. Although the external-electric-field-based self-assembly (EEFSA) strategy for decreasing NMNP gap in liquid phase is relatively developed, it is rarely described in solid phase. Here, by combining corona discharge technique (CDT) as a simple EEFSA approach on flexible substrate surface modification, a flexible SERS substrate medicated with gold nanospheres (AuNSs) is produced. Because of the CDT's peculiar discharge event, makes AuNSs aggregation simply achieved. The modified flexible SERS substrate is sensitive to the detection limit of ∼10-5 mM for Rhodamine 6G (R6G), with a maximum enhancement factor of 2.79×106. Furthermore, finite-difference time-domain (FDTD) simulation confirms the SERS enhancement impact of AuNSs-based substrate. This study not only provides a low-cost, simple-to-process, high-yield, high sensitivity, and activity flexible SERS substrate, but also suggests a more practical and adaptable NMNPs self-assembly approach.