Although gold nanorods (GNRs) have been prepared with a wide range of methods for their uses as novel diagnostic and therapeutic agents, the synthesis of monodispersed GNRs with high yields and size tunability still requires further improvements. We report on a simple one-pot method for preparing highly monodispersed GNRs using phenols (e.g., hydroquinone, 1,2,3-trihydroxybenzene, and 1,2,4-trihydroxybenzene) as the reducing agent and NaBH<inf>4</inf> as the initiating reactant. Fine-tuning of the LSPR peak position of phenols-reduced GNRs from 550 to 1150 nm is accomplished by regulating the silver ion concentrations. The size of GNRs produced via phenols reduction can also be controlled by changing the NaBH<inf>4</inf> concentration. By systematically optimizing the concentrations of the reagents involved in the one-pot synthesis of GNRs, the yield (in many cases exceeding 90%) is significantly higher than that prepared with the commonly used reductant (e.g., ascorbic acid). The improved efficiency and controllability cut down the cost and time involved in GNRs production. ©2014 American Chemical Society.