Synchrotron x-ray diffraction and high-resolution electron microscopy revealed the origin of different strain hardening behaviors (and dissimilar tensile ductility) in nanocrystalline Ni and nanocrystalline Co. Planar defect accumulations and texture evolution were observed in Co but not in Ni, suggesting that interfacial defects are an effective passage to promote strain hardening in truly nanograins. Twinning becomes less significant in Co when grain sizes reduce to below ~15 nm. This study offers insights into achieving excellent mechanical properties in nanocrystalline materials.