We report the electron-spin polarization of D atoms from the photodissociation of DI, at 213 nm and 266 nm, by measuring the magnetization quantum beats of the D atoms with a pick-up coil. We determine that the polarization P is large at both wavelengths (|P|∼ 1), however it is positive at 213 nm, and negative at 266 nm. These results, in both cases, are of opposite sign to calculations, which assume adiabatic dissociation along the A1Π1 or a3Π1 states. We interpret these results as evidence that nonadiabatic coupling between these states needs to be included for the theoretical treatment of DI photodissociation.