Nanofibrous materials composed of polyesters play a key role in several technologically demanding fields, most notably that of biomedicine. A critical feature of polyesters is their ability to tune mechanical properties through simple blending of components. This work explores the fabrication of blended poly(lactic acid)/poly(epsilon-caprolactone) (PLA/PCL) fibers manufactured through multilayer coextrusion. Morphology, crystallinity, and crystallite size were probed for a continuum of blends to understand the resultant mechanics of the nanofibers. Fibers with differential weight ratios displayed a droplet-in-matrix morphology (75/25 PLA/PCL; 25/75 PLA/PCL), whereas 50/50 PLA/PCL blends exhibited a cocontinuous morphology. Depression of the crystallinity of both phases was observed for all blends and changes in the mean crystallite size typically decreased upon blending. The microscale behavior of the materials explains the tensile properties of the fibers; mechanical analysis showed that the addition of PCL increased the extensibility and toughness, in particular, for blends that formed a cocontinuous morphology. Correlating morphological effects on the crystallinity and mechanics of melt-processed fibers provides insight into the interaction between two semicrystalline phases and provides valuable insight for future technological development.