Biosorption is a cost-effective and simple technique for removing heavy metals and rare earth elements from aqueous solution. Here, metals were recovered from aqueous solutions using phosphorylated dry baker’s yeast cells. The cells were phosphorylated using cyclo-triphosphate, Na3P3O9. The total P content of the phosphorylated cells was ~1.0 mmol/g dry cell weight (DCW). The zeta potential of the phosphorylated cells was −45 mV, two times higher than for the non-phosphorylated cells. The strong negative charges of the phosphorylated cells allowed the cells to adsorb heavy metal ions such as Cd2+, Cu2+, Pb2+, and Zn2+, the adsorption capacities of which reached ~1.0 mmol/g DCW. This adsorption capacity was the highest level found in the previous studies using yeast dead biomass. The adsorbed metal ions were easily desorbed in 0.1 M HCl. The phosphorylated cells also adsorbed rare earth ions including Ce3+, Dy3+, Gd3+, La3+, Nd3+, Y3+, and Yb3+ with high efficiency. Furthermore, the phosphorylated yeast cells selectively adsorbed the rare earth ions (Nd3+ and Yb3+) from a solution containing heavy metals and rare earth ions because trivalent positively charged ions were adsorbed preferentially over divalent ions. Thus, phosphorylated yeast cells therefore have great potential for use as novel bioadsorbents. It is also expected that this technique can be applied to many microbial materials as well as yeast.