A richly structured luminescence is observed in the 1.2-pm spectral region in "pure" and Fedoped ZnS crystals for the first time. By means of emission, excitation, and magneto-optical measurements an unambiguous assignment to the Tl (G)-A 1(S) transition of isolated Fe + on Zn + lattice sites becomes possible. Basic arguments are the sixfold degeneracy of the ground state with an isotropic g factor of 2.026+0.010, the long decay time of about 4 ms, and the influence of additional iron doping. The excitation mechanism can be described by an energy transfer via free holes from hC u + to Fe' centers and a charge-transfer process Fe':Fe'++Ave (VB denotes valence band). A comparison with the well-known isoelectronic Mn + centers reveals striking similarities.The numerous zero-phonon lines at T =1.8 K are due to the polytypic structure of the investigated crystals, offering several different Zn' lattice sites. The observed fine structures of the Tl(G) terms and their behavior in a magnetic field indicate a strong Jahn-Teller coupling to E modes as is known for the Mn + centers.