Focusing on nanocrystalline (nc) pure face-centered cubic metals, where systematic experimental data are available, this paper presents a brief overview of the recent progress made in improving mechanical properties of nc materials, and in quantitatively and mechanistically understanding the underlying mechanisms. The mechanical properties reviewed include strength, ductility, strain rate and temperature dependence, fatigue and tribological properties. The highlighted examples include recent experimental studies in obtaining both high strength and considerable ductility, the compromise between enhanced fatigue limit and reduced crack growth resistance, the stress-assisted dynamic grain growth during deformation, and the relation between rate sensitivity and possible deformation mechanisms. The recent advances in obtaining quantitative and mechanics-based models, developed in line with the related transmission electron microscopy and relevant molecular dynamics observations, are discussed with particular attention to mechanistic models of partial/perfect-dislocation or deformation-twin-mediated deformation processes interacting with grain boundaries, constitutive modeling and simulations of grain size distribution and dynamic grain growth, and physically motivated crystal plasticity modeling of pure Cu with nanoscale growth twins. Sustained research efforts have established a group of nanocrystalline and nanostructured metals that exhibit a combination of high strength and considerable ductility in tension. Accompanying the gradually deepening understanding of the deformation mechanisms and their relative importance, quantitative and mechanisms-based constitutive models that can realistically capture experimentally measured and grain-size-dependent stress–strain behavior, strain-rate sensitivity and even ductility limit are becoming available. Some outstanding issues and future opportunities are listed and discussed.