We report the highest-energy observation of entanglement, in top−antitop quark events produced at the Large Hadron Collider, using a proton−proton collision data set with a center-of-mass energy of $\sqrt{s}=13$ TeV and an integrated luminosity of 140 fb$^{−1}$ recorded with the ATLAS experiment. Spin entanglement is detected from the measurement of a single observable $D$, inferred from the angle between the charged leptons in their parent top- and antitop-quark rest frames. The observable is measured in a narrow interval around the top−antitop quark production threshold, where the entanglement detection is expected to be significant. It is reported in a fiducial phase space defined with stable particles to minimize the uncertainties that stem from limitations of the Monte Carlo event generators and the parton shower model in modelling top-quark pair production. The entanglement marker is measured to be $D=−0.537\pm 0.002 (\text{stat.})\pm 0.019 (\text{syst.})$ for $340<m_{t\bar{t}}<380$ GeV. The observed result is more than five standard deviations from a scenario without entanglement and hence constitutes both the first observation of entanglement in a pair of quarks and the highest-energy observation of entanglement to date.