Cu/Ni multilayers with various defined thickness of Cu and Ni layers were electrodeposited on low carbon steel substrates. Hardness measurements indicated that the increase in yield strength (one-third of hardness) with a decrease of layer thickness for Cu/Ni multilayers with single layer thickness at sub-micron length scale could be described by the Hall-Petch formula of the dislocation pile-up model. In the regime of few tens to a hundred nanometers of single layer thickness, the dislocation pileup-based Hall-Petch model broke down. This could be explained quantitatively according to the criterion condition on the limit size of dislocation derived from a modified Thomas-Fermi-Dirac electron theory.