The current work investigates the four-wave mixing (FWM) signal from gold nanorods (NRs) using two synchronized lasers and its potential applications in bioimaging. Using the lightning rod model, we show that the strongest FWM occurs when the pump laser wavelength is tuned to be resonant with the longitudinal plasmon resonance wavelength of NR. The calculation is experimentally demonstrated by comparing the intensities of FWM from NRs with different plasmon resonance wavelengths. The FWM signal is further found to be enhanced by aggregation of NRs and is strongly dependent on pulse width. The FWM intensity from NRs is ∼39 times stronger than the coherent anti-Stokes Raman scattering intensity from melamine beads. This plasmon-resonance-enhanced FWM signal enables NRs to be used as a nonlinear optical (NLO) imaging probe.