Molybdenum (Mo) is critical for the function of enzymes related to nitrogen cycling. Concentrations of Mo are very low in sandy, acidic soils, and biologically available Mo is only a small fraction of the total pool. While several methods have been proposed to measure plant-available Mo, there has not been a recent comprehensive analytical study that compares soil extraction methods as predictors of plant Mo uptake. A suite of five assays [total acid microwave digestion, ethylenediamenetetraaacetic acid (EDTA) extraction, Environmental Protection Agency (EPA) protocol 3050B, ammonium oxalate extraction, and pressurized hot water] was employed, followed by the determination of soil Mo concentrations via inductively coupled mass spectroscopy. The concentrations of soil Mo determined from these assays and their relationships as predictors of plant Mo concentration were compared. The assays yielded different concentrations of Mo: total digest > EPA > ammonium oxalate ≥ EDTA > pressurized hot water. Legume foliar Mo concentrations were most strongly correlated with ammonium oxalate–extractable Mo from soils, but an oak species showed no relationship with any soil Mo fraction and foliar Mo. Bulk fine roots in the 10- to 30-cm soil horizon were significantly correlated with the ammonium oxalate Mo fraction. There were significant correlations between ammonium oxalate Mo and the oxides of iron (Fe), manganese (Mn), and aluminum (Al). Results suggest that the ammonium oxalate extraction for soil Mo is the best predictor of plant-available Mo for species with high Mo requirements such as legumes and that plant-available Mo tracks strongly with other metal oxides in sandy, acidic soils.