Gold nanorods (AuNRs) with different aspect ratios were prepared by the seed-mediated growth method and combined with three carbon-based nanomaterials of multiple dimensions (i.e., zero-dimensional (0D) carbon black (CB), onedimensional (1D) carbon nanotubes (CNTs), and two-dimensional (2D) graphene oxide (GO)). The AuNR/carbon-based nanomaterial hybrids were utilized in dynamic surface-enhanced Raman scattering (D-SERS). First, cetyltrimethylammonium bromide (CTAB) was used to stabilize and coat the AuNRs, enabling them to be dispersed in water and conferring a positive charge to the surface. AuNR/carbon-based nanomaterial hybrids were then formed via electrostatic attraction with the negatively charged carbon-based nanomaterials. Subsequently, the AuNR/carbon-based nanomaterial hybrids were utilized as large-area and highly sensitive Raman spectroscopy substrates. The AuNR/GO hybrids afforded the best signal enhancement because the thickness of GO was less than 5 nm, which enabled the AuNRs adsorbed on GO to produce a good three-dimensional hotspot effect. The enhancement factor (EF) of the AuNR/GO hybrids for the dye molecule Rhodamine 6G (R6G) reached 1 × 10 7 , where the limit of detection (LOD) was 10 −8 M. The hybrids were further applied in D-SERS (detecting samples transitioning from the wet state to the dry state). During solvent evaporation, the system spontaneously formed many hotspots, which greatly enhanced the SERS signal. The final experimental results demonstrated that the AuNR/GO hybrids afforded the best D-SERS signal enhancement. The EF value for R6G reached 1.1 × 10 8 after 27 min, with a limit of detection of 10 −9 M at 27 min. Therefore, the AuNR/GO nanohybrids have extremely high sensitivity as molecular sensing elements for SERS and are also very suitable for the rapid detection of single molecules in water quality and environmental management.