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Using a total of 5.25 fb−1 of e+e− collision data with center-of-mass energies from 4.236 to 4.600 GeV, we report the first observation of the process e+e− → ηψ(2S) with a statistical significance of 4.9 standard deviations. The data sets were collected by the BESIII detector operating at the BEPCII storage ring. We measure the yield of events integrated over center-of-mass energies and also present the energy dependence of the measured cross section.