Gold nanorods (AuNRs) have shown great potentials in biological and biomedical application such as molecular imaging, drug delivery, or photothermal therapy. The optical properties of these elongated nanoparticles depend on their shape anisometry. The AuNR-based longitudinal localized surface plasmon resonance (longitudinal LSPR) band is very sensitive to the AuNR’s aspect ratio and the surrounding local environment. We investigate for the first time with a pulse-shaper-based two-dimensional electronic spectroscopy (2DES) to study these noble metal nanoparticles.