Mo isotope compositions have been increasingly used as a source tracer in magmatic systems. Here, we investigate the relative role of subducting oceanic crust, fluid-rich sources (e.g., serpentinite, altered oceanic crust – AOC), subducted sediments and upper mantle in the chemical composition of Aleutian arc magmas with Mo and B systematics. We present elemental and Mo isotope compositions (δ98/95Mo) and B concentrations on Aleutian lavas (n = 59), from Okmok Volcano in the east to the westernmost seamount Piip, showing absence of Mo isotope fractionation during magmatic differentiation. Additionally, we report Mo isotope systematics for serpentinized peridotites from the South-West Indian Ridge (SWIR) (n = 6), AOC (n = 2) and Pacific sediments (DSDP 183, ODP 886) (n = 5) outboard the Aleutian arc. Molybdenum isotope composition and B enrichment (e.g., B/Ce) patterns display a step-function increase along the arc, with low, MORB-like, δ98/95Mo and low B/Ce values in the western section of the arc (B/Ce = 0.15–1.07; δ98/95Mo =−0.38 to +0.01‰), that abruptly increase in the central-eastern volcanoes Korovin, Seguam and Yunaska (B/Ce = 1.20–2.60; δ98/95Mo = +0.03 to +0.30‰) near the intersection of the Amlia Fracture Zone (AFZ) with the trench, but decrease again farther east at Okmok (B/Ce = 0.76 and δ98/95Mo = −0.12‰ on average). These data patterns are interpreted to reflect an along-arc changing source in the Aleutian magmas. AOC and Pacific sediments have predominantly low δ98/95Mo (−0.47 to −0.32 and +0.17 to −1.9‰, respectively), while serpentinites have extremely high δ98/95Mo (up to +1.09‰) and high B/Ce (∼22000). Based on the low δ98/95Mo in sediments and AOC, and lack of correlation between along-arc δ98/95Mo and radiogenic sediment tracers, subducted sediments and AOC do not exert first-order controls on the observed Mo isotope compositions. Rather, low, MORB-like, δ98/95Mo but high Mo enrichments (e.g., Mo/Ce) in the western samples are consistent with slab melting under rutile-bearing eclogitic facies with near absent Mo isotope fractionation from the slab to the arc sources. In turn, the abrupt increase of δ98/95Mo and B/Ce in lavas near the AFZ are best explained by a serpentinite endmember (likely dehydration fluids) at the AFZ that is not evident elsewhere along the arc. Results from this study provide evidence for serpentinites as an additional heavy Mo isotope signature component in subduction zones and demonstrate that high δ98/95Mo coupled with B enrichments are a useful proxy for tracing serpentinite fluids in subduction zones.