We present a neutron scattering investigation of Ce1-xYxAl3 as a function of chemical pressure, which induces a transition from heavy-fermion behavior in CeAl3 (TK=5 K) to a mixed-valence state at x=0.5 (TK=150 K). The crossover can be modeled accurately on an absolute intensity scale by an increase in the k-f hybridization, Vkf, within the Anderson impurity model. Surprisingly, the principal effect of the increasing Vkf is not to broaden the low-energy components of the dynamic magnetic susceptibility but to transfer spectral weight to high energy.