The size dependence of strength observed in submicrometer face-centered-cubic (fcc) metallic crystals under uniform deformation depends on the interaction of pre-existing dislocations with surfaces. To date, however, the dislocation processes controlling flow stress scaling in fcc crystals less than 100 nm in size have remained an open question due to limited knowledge on microstructural evolution during deformation in such small volumes. Here, molecular dynamics computer simulations employing a technique of high-temperature annealing and quenching on porous crystals were used to generate complex dislocation microstructures in sub-75 nm Cu pillars with high initial dislocation densities of 10 16 m −2, which made it possible to quantitatively examine their evolution during compression as a function of pillar diameter. These simulations reveal a transition from a state of dislocation exhaustion, where mobile dislocations are lost at the free surface and the dislocation density steadily decreases, to a regime of intermittent plastic flow between elastic loading and source-limited activation inside the pillars. It is shown that plastic flow stresses predicted during dislocation exhaustion regime exhibit little to no size dependence, while pronounced size effects are found during source-limited activation. Remarkably, the relationship between flow stress predicted at 5% strain and diameter is found to follow closely the power-law dependence reported in past experiments with larger Cu crystals and smaller densities. A deformation mechanism map, expressed in terms of diameter, is developed and used to elucidate the origin of size-dependent plasticity in nanoscale fcc crystals.