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Entanglement is a key property of quantum systems. In this Letter the first measurements of quantum entanglement between spins in pairs of Z bosons are reported, using proton-proton collision data from the Large Hadron Collider (LHC) at center-of-mass energies of 13 and 13.6 TeV, recorded with the ATLAS detector. Measurements of angular observables sensitive to ZZ^{*} spin-density-matrix elements in the H→ZZ^{*}→ℓ^{+}ℓ^{-}ℓ^{+}ℓ^{-} process yield coefficients C_{2,1,2,-1}=-0.71±0.45 and C_{2,2,2,-2}=0.08±0.44, consistent with their Standard Model predictions. A complementary hypothesis test using the full angular distribution, and relying on several Standard Model assumptions in the decays, provides substantially higher sensitivity to quantum correlations and disfavors the separable-state hypothesis at a significance of 4.7 standard deviations (expected 4.9σ) relative to the entangled Standard Model hypothesis. These results provide strong evidence of quantum entanglement between massive bosons (spin qutrits) at the electroweak scale.