We present differences in the mechanical behavior of nanoscale gold and molybdenum single crystals. A significant strength increase is observed as the size is reduced to 100 nm. Both nanocrystals exhibit discrete strain bursts during plastic deformation. We postulate that they arise from significant differences in the dislocation behavior. Dislocation starvation is the predominant mechanism of plasticity in nanoscale fcc crystals, while junction formation and hardening characterize bcc plasticity. A statistical analysis of strain bursts is performed as a function of size and compared with stochastic models. DOI: 10.1103/PhysRevLett.100.155502 PACS numbers: 62.25.ÿg, 61.46.Hk, 81.07.ÿb, 81.16.Rf The mechanical behavior of crystals is dictated by dislocation motion in response to applied force. While it is difficult to observe the motion of individual dislocations, several correlations can be made between the microscopic stress-strain behavior and dislocation activity. In bulk, plasticity in metals occurs by the motion of dislocations, which multiply in the course of plastic deformation causing strain hardening. Although this fundamental concept is often assumed to be applicable to crystals of any dimensions, numerous recent studies have shown that conventional plasticity breaks down at the submicron scale. Recently, many experimental and computational investigations of fcc crystals (Au, Al, Cu, Ni) have demonstrated a pronounced size effect, whose main premise is ''smaller is stronger '' [1-11]. In this work we investigate flow stress as a function of diameter in gold (fcc) and molybdenum (bcc) single crystal nanopillars subjected to uniaxial microcompression. The results that follow suggest that fcc and bcc crystals have fundamentally different plasticity mechanisms when reduced to nanoscale with significant strain hardening present in the latter and virtually none in the former. In a striking deviation from classical mechanics, there is a significant increase in strength as crystal size is reduced to 100 nm; however, in gold crystals (fcc) the highest strength achieved represents 44% of its theoretical strength, while in molybdenum crystals (bcc) it is only 7%. This suggests that plasticity in Au is likely controlled by nucleation of new dislocations rather than by interactions of the preexisting ones. On the contrary, the smallest molybdenum nanopillar achieves only 7% of its theoretical strength, implying that plasticity is likely driven by the intricate motion and interactions of dislocations inside the pillar rather than by nucleation events. These remarkable differences in mechanical response of fcc and bcc crystals to uniaxial microcompression challenge the applicability of conventional strain hardening to nanoscale crystals. Single crystal nanopillars described in this work were fabricated via the focused ion beam system and subsequently uniaxially compressed along the h001i direction in the nanoindenter with a flat punch tip of 30 m diameter. The specifics of fabrication and testing conditions are b...