Trace elements, including rare earth elements (REE), exhibit systematic variations in plutonic rocks from the Captains Bay pluton which is zoned from a narrow gabbroic rim to a core of quartz monzodiorite and granodiorite. The chemical variations parallel those in the associated Aleutian calcalkaline volcanic suite. Concentrations of Rb, Y, Zr and Ba increase as Sr and Ti decrease with progressive differentiation. Intermediate plutonic rocks are slightly enriched in light REE (La/Yb=3.45-9.22), and show increasing light REE fractionation and negative Eu anomalies (Eu/Eu*=1.03-0.584). Two border-zone gabbros have similar REE patterns but are relatively depleted in total REE and have positive Eu anomalies; indicative of their cumulate nature. Initial 87Sr/86Sr ratios in 8 samples (0.70299 to 0.70377) are comparable to those of volcanic rocks throughout the arc and suggest a mantle source for the magmas. Oxygen isotopic ratios indicate that many of the intermediate plutonic rocks have undergone oxygen isotopic exchange with large volumes of meteoric water during the late stages of crystallization; however no trace element or Sr isotopic alteration is evident. Major and trace element variations are consistent with a model of inward fractional crystallization of a parental high-alumina basaltic magma at low pressures (〈6 kb). Least-squares approximations and trace element fractionation calculations suggest that differentiation in the plutonic suite was initially controlled by the removal of calcic plagioclase, lesser pyroxene, olivine and Fe-Ti oxides but that with increasing differentiation and water fugacity the removal of sub-equal amounts of sodic plagioclase and hornblende with lesser Fe-Ti oxides effectively drove residual liquids toward dacitic compositions. Major and trace element compositions of aplites which intrude the pluton are not adequately explained by fractional crystallization. They may represent partial melts derived from the island arc crust. Similarities in Sr isotopes, chemical compositions and differentiation trends between the plutonic series and some Aleutian volcanic suites indicates that shallow-level fractional crystallization is a viable mechanism for generating the Aleutian calcalkaline rock series.