Three-dimensional plasma nanostructures with high light–thermal conversion efficiency show the prospect of industrialization in various fields and have become a research hotspot in areas of light–heat utilization, solar energy capture, and so on. In this paper, a simple chemical synthesis method is proposed to prepare gold nanoparticles, and the electrophoretic deposition method is used to assemble large-area three-dimensional gold nanostructures (3D-GNSs). The light–thermal water evaporation monitoring and surface-enhanced Raman scattering (SERS) measurements of 3D-GNSs were performed via theoretical simulation and experiments. We reveal the physical processes of local electric field optical enhancement and the light–thermal conversion of 3D-GNSs. The results show that with the help of the efficient optical trapping and super-hydrophilic surface properties of 3D-GNSs, they have a significant effect in accelerating water evaporation, which was increased by nearly eight times. At the same time, the three-dimensional SERS substrates based on gold nanosphere particles (GNSPs) and gold nanostar particles (GNSTs) had limited sensitivities of 10⁻¹⁰ M and 10⁻¹² M to R6G molecules, respectively. Therefore, 3D-GNSs show strong competitiveness in the fields of solar-energy-induced water purification and the Raman trace detection of organic molecules.