The 4.509-MeV state in 21Al has been investigated using the 26Mg(p, γ) reaction at the Ep = 2.174-MeV resonance. On the basis of γ-ray angular distributions, the spin–parity assignment of the resonance (Ex = 10.366 MeV) is found to be 7/2+ and strong evidence is given that the 4.509-MeV state in 27Al has Jπ = 11/2+. The lifetime is found to be τ(4.509) = 340 fs ± 10%. The 8.040-MeV state in 27Al has a spin–parity assignment of 7/2+. Branching ratios are given for the resonance as well as levels above the 4.509-MeV state fed by the resonance.