Uniaxial tensile tests were performed on high-purity nickel polycrystals with thicknesses (t) ranging from 12.5 to 3200 μm. The grain size (d) of each sample was set to a value close to 100 μm in order to avoid grain size effects. Experimental results highlight the intrinsic effect of the thickness on the mechanical properties of nickel. For plastic strains higher than 0.01, a strong softening of the flow stress is clearly observed when the t/d ratio decreases from four to one. This critical range is independent of the plastic strain. Transmission electron microscopy (TEM) investigations of dislocation structures were carried out in core and surface regions of samples plastically strained in the second hardening stage. It is shown that the mean dislocation cell diameter obtains values two or three times higher near free surfaces than in core areas for specimens with t/d ratios lying at a range of 1 to 4. This observation can be interpreted in terms of an increase in the mean free path of mobile dislocations in the second hardening stage. The transition between polycrystal and single-crystal behavior for nickel with constant grain size and various thicknesses is, therefore, an intrinsic effect related to progressively stronger surface softening effects.