Tailoring the longitudinal surface plasmon wavelengths (LSPWs), scattering, and absorption cross sections of gold nanorods has been demonstrated by combining anisotropic shortening and transverse overgrowth and judiciously choosing starting Au nanorods. Shortening yields Au nanorods with decreasing lengths but a fixed diameter, while overgrowth produces nanorods with increasing diameters but a nearly unchanged length. Two series of Au nanorods with LSPWs varying in the same spectral range but distinct extinction coefficients are thus obtained. The systematic changes in the LSPW and extinction for the two series of Au nanorods are found to be in good agreement with those obtained from Gans theory. Dark-field imaging performed on two representative nanorod samples with similar LSPWs shows that the scattering intensities of the overgrown nanorods are much larger than those of the shortened nanorods. The experimental results are found to be in very good agreement with those obtained from finite-difference time-domain (FDTD) calculations. FDTD calculations further reveal that the scattering-to-extinction ratio increases linearly as a function of the diameter for Au nanorods with a fixed aspect ratio.