The spectrum and size controllable synthesis of gold nanorods is of great value for their widely applicable aspect ratio dependence of anisotropic surface plasmon resonance. Herein, 1,7-dihydroxynaphthalene with a relatively strong reducibility is proposed as a reducing agent for the controllable synthesis of gold nanorods. The result indicated that gold nanorods with high monodispersity, high shape yield, relatively small diameters, and maximum plasmon resonance wavelength of above 1000 nm can be acquired. More importantly, by virtue of the reducing agent used, fine and precise controls over the plasmon wavelength and diameter of the rod can be achieved via changes in experimental conditions. In particular, increases in the concentration of both silver ions and cetyltrimethylammonium bromide (CTAB) can increase the plasmon wavelength from around 600 nm to 1000 nm but respectively show a decreased diameter with the smallest value of around 14.3 nm and a mildly increased diameter from around 9.0 nm to 14.3 nm; moreover, increasing the concentration of reducing agents and gold seeds can simultaneously cause decreases in the plasmon wavelength from around 1000 nm to 800 nm and the diameters from around 14.3 nm to 9.0 and 7.3 nm, respectively. This powerful and efficient method of controllable synthesis of AuNRs could be valuable and attractive for the application of the as-obtained particles.