This Letter reports a measurement of the exclusive γγ→ℓ+ℓ− ( ℓ=e, μ ) cross-section in proton–proton collisions at a centre-of-mass energy of 7 TeV by the ATLAS experiment at the LHC, based on an integrated luminosity of 4.6 fb−1 . For the electron or muon pairs satisfying exclusive selection criteria, a fit to the dilepton acoplanarity distribution is used to extract the fiducial cross-sections. The cross-section in the electron channel is determined to be σγγ→e+e−excl.=0.428 ± 0.035 (stat.) ± 0.018 (syst.) pb for a phase–space region with invariant mass of the electron pairs greater than 24 GeV , in which both electrons have transverse momentum pT>12 GeV and pseudorapidity |η|<2.4 . For muon pairs with invariant mass greater than 20 GeV , muon transverse momentum pT>10 GeV and pseudorapidity |η|<2.4 , the cross-section is determined to be σγγ→μ+μ−excl.=0.628 ± 0.032 (stat.) ± 0.021 (syst.) pb . When proton absorptive effects due to the finite size of the proton are taken into account in the theory calculation, the measured cross-sections are found to be consistent with the theory prediction.