The compositional variability of ocean island basalts (OIBs) is thought to reflect partial melting of a lithologically-heterogeneous mantle source dominated by either pyroxenite or peridotite. The Pohnpei Island in Micronesia, which is associated with the Caroline hotspot, is suggested to have been generated from partial melting of a pyroxenite-rich mantle. To examine this hypothesis, we present new major- and trace-element compositions of olivine phenocrysts in basalts from the island. The olivines exhibit large systematic inter- and intra-crystalline compositional variability. In Sample DS1, olivines record compositional zonation, in which cores have relatively high Fo (77–85), Ni (550×10?6–2392×10?6), and Fe/Mn ratios (66–82), whereas rims have lower Fo (71–78), Ni (526×10?6–1537×10?6), and Fe/Mn ratios (51–62). By contrast, olivines within other samples preserve no clear compositional zonation, exhibiting similar or slightly lower Fo values (66–78), Ni contents (401×10?6–1268×10?6), and Fe/Mn ratios (53–69) as the rims of zoned crystals. The distinct chemical contrast between the two different types of olivine suggests they formed in magma chambers at different depths. Analysis using forward petrological modeling and multi-element indicators (Fe/Mn, Zn/Fe, FC3MS (FeOT/CaO?(3×MgO/SiO2)), Mn/Zn, and Ni/(Mg/Fe)) of whole-rock samples and high-Fo olivines is inconsistent with a pyroxenite-rich mantle source. We suggest these inconsistencies reflect an influence on the partition coefficients of Ni and Mn between olivine and liquid during melting at variable pressures and temperatures. In addition, magma recharge and mixing within the magmatic plumbing system can change the composition of olivine. We suggest that identification of the mantle source of OIBs in volcanic islands such as the Pohnpei Island using olivine geochemistry should be treated with caution.