The exceptional strength and distinct deformation physics exhibited by pure ultrafine-grained and nanocrystalline metals in comparison to their microcrystalline counterparts have been ascribed to the dominant influence of grain boundaries in accommodating plastic flow. Such grain-boundary-mediated mechanisms can be augmented by additional strengthening in nanocrystalline alloys via solute and precipitate interactions with dislocations, although its potency is a function of the changes in the elastic properties of the alloyed material. In this study, we investigate the elastic and plastic properties of Al1−xMox alloys (0⩽x⩽0.32) by tensile testing of sputter-deposited freestanding thin films. Isotropic elastic constants and strength are measured over the composition range for which three microstructural regimes are identified, including solid solutions, face-centered cubic and amorphous phase mixtures and body-centered cubic (bcc)/amorphous mixtures. Whereas the bulk modulus is measured to follow the rule of mixtures over the Mo composition range, the Young’s and shear moduli do not. Poisson’s ratio is non-monotonic with increasing Mo content, showing a discontinuous change at the onset of the bcc/amorphous two-phase region. The strengthening measured in alloyed thin films can be adequately predicted in the solid solution regime only by combining solute strengthening with a grain boundary pinning model. The single-step co-sputtering procedure presented here results in diversity of alloy compositions and microstructures, offering a promising avenue for tailoring the mechanical behavior of thin films.