Nanocracks can generate at the intersection of the deformation twin and grain boundary (GB). A mathematical model is built to study the nanoinhomogeneity effect on nanocrack nucleation and propagation in the nanocrystalline matrix. The boundary condition at the interface between the nanoinhomogeneity and the matrix is modified by incorporating the interface effect. The influence of the nanoinhomogeneity shear modulus, the nanoinhomogeneity radius, the nanoinhomogeneity position, the interface effect, and the external stress on the nanocrack nucleation and propagation is investigated in detail. The results indicate that the stiff nanoinhomogeneity suppresses nanocrack nucleation and propagation and thereby improves the tensile ductility of nanocomposites without loss of their predominantly high strength. Both the positive interface residual tension and interface elastic constants suppress nanocrack nucleation and propagation, while the negative interface residual tension and interface elastic constants promote nanocrack nucleation and propagation. Furthermore, the effect of interface residual tension is rather significant. The interface elastic constants have a weak effect on nanocrack nucleation and propagation.