In order to gain a fundamental understanding of the deformation behavior of multilayer architectures composed of a periodic layering of hard and soft structural features, NiCo samples possessing modulated nanocrystalline and coarse-grained microstructures were fabricated using pulsed electrodeposition. Scanning electron microscopy imaging confirmed that the samples possessed an alternating grain size distribution and the desired 1:1 thickness ratio of constitutive layers. Uniaxial tensile testing showed a rule of mixtures relationship in yield and ultimate tensile strengths for the multilayer with respect to reference samples. Notably, an increase in elongation to failure was observed in the multilayer when compared to the nanocrystalline reference. The gains in elongation were found to be associated with improved neck stability due to dislocation activity within the coarse-grained layers. The morphology of the fracture surface, considered together with the available mechanical data, electron micrographs and texture measurements, forms the basis of a multiscale deformation mechanism which describes a failure pathway for multilayer architectures with nanocrystalline and coarse-grained structural features.