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The intermediate-valence compound CeNi experiences a pressure-induced first-order structural phase transition with an abrupt change in the unit cell volume, and as such constitutes an attractive system to study pressure-driven f-electron delocalization behavior in a system with an unstable f-electron shell. The inelastic neutron scattering study of the dynamic magnetic response of CeNi reveals that the structural transition increases the characteristic energy of magnetic fluctuations due to enhanced Ce 4f–Ni 3d hybridization. At the same time, the inelastic 4f magnetic form factor remains unchanged.