The radiotracer technique was applied for measuring grain boundary diffusion of Ni in ultrafine grained (UFG) copper materials with different nominal purities and in a Cu—1wt.%Pb alloy. The UFG specimens were prepared by equal channel angular pressing at room temperature. The stability of the microstructure was studied by focused ion beam imaging. Grain boundary diffusion of the 63Ni radioisotope was investigated in the temperature interval from 293 to 490K under the formal Harrison type C kinetic conditions. Two distinct short-circuit diffusion paths were observed. The first (relatively slow) path in the UFG materials corresponds unambiguously to relaxed high-angle grain boundaries with diffusivities which are quite similar to those in the respective coarse-grained reference materials. The second path is characterized by significantly higher diffusivities. The experimental data are discussed to elucidate the contribution of nonequilibrium grain boundaries in the deformed materials. Alternative contributions of other shortcircuit diffusion paths cannot be ruled out, particularly for the Cu-Pd alloy.