While extensive research has been dedicated to plasmon tuning within non-noble metals, prior investigations primarily concentrated on markedly augmenting the inherently low concentration of free carriers in materials with minimal consideration given to the influence of electron orbitals on surface plasmons. Here, we achieve successful intercalation of Au atoms into the layered structure of Fe3GeTe2 (FGT), thereby exerting control over the orbital electronic states or structure of FGT. This intervention not only amplifies the charge density and electron mobility but also mitigates the loss associated with interband transitions, resulting in increased two-dimensional FGT surface plasmon activity. As a consequence, Au-intercalated FGT detects crystal violet molecules as a surface-enhanced Raman scattering substrate, and the detection lines are 3 orders of magnitude higher than before Au intercalation. Our work provides insight for further studies on plasmon effects and the relation between surface plasmon resonance behavior and electronic structures.