The α–γ angular correlation of the cascade Bi211(α, 6.27 MeV)Tl207*(γ, 350 keV)Tl207 has been found to be isotropic to within [Formula: see text].Accepting the spin and parity of the ground state of Tl207as 1/2+, a search was made for all reasonable spins and angular momenta, pure and mixed, which could yield an isotropic correlation. Shell-model predictions and other situations have been examined. No case of unmixed α-, unmixed γ-angular momenta satisfies the isotropy condition. Many other cases are found which do so, but only with the spin and parity of the excited state of Tl207 taken as 3/2+. It has been shown that 5/2+ does not yield an isotropic correlation. With one radiation mixed and the other pure, there are eight possible combinations which fit the observations. With both radiations mixed, there is an infinity of combinations of the two mixing parameters which lead to an isotropic distribution. The αk value of the 350-keV transition (0.175 ± 0.017) shows the γ ray in question to be 76% M1 and 24% E2. The present work is consistent with only one of the two possibilities given by Gorodetzky et al. (1962) from polarization–correlation work. Accepting this additional evidence it would appear that the most plausible interpretation is that of shell-model spins and parities with both radiations mixed, α—(λ = 3, 5), γ—(76% M1, 24% E2).