In vivo and in vitro studies were carried out to characterize the exchangeable bone magnesium pool and determine what effect age and magnesium depletion has on bone magnesium. A highly significant correlation was found between the size of the in vitro elutable and in vivo exchangeable bone magnesium (r = 0.97). To show that the exchangeable bone magnesium was the surface limited bone magnesium, elution studies were performed 4 h after the in vivo administration of radiomagnesium. Specific activity in the eluant was 85% of that found in the serum at time of death, suggesting that the elutable and exchangeable bone magnesium pools were largely the same pool. Bone magnesium concentration fell with increasing age. The entire fall in bone magnesium was a result of a decrease in the surface limited fraction. Since bone crystals have been shown to enlarge with aging with resulting contraction of the surface area, this would be the most apparent explanation for this finding. During magnesium depletion, magnesium concentration in both the exchangeable and nonexchangeable pools decreased. The fractional change in the exchangeable pool was much larger than the change in total or nonexchangeable bone magnesium, suggesting that the surface limited magnesium pool is available during magnesium depletion. The change in size of the nonexchangeable bone magnesium pool appeared to be more related to the duration of magnesium depletion than the change in serum magnesium levels. The fall in magnesium concentration in this pool is probably a consequence of continuing formation of low magnesium bone during the depletion period.