Strengthening of alloys can be efficiently attained by the creation of harmonic structures: bimodal microstructures generated by controlled milling of the particulate precursors, which consist of coarse-grained cores embedded in a continuous fine-grained matrix. Here, we extend the concept of harmonic structures to metal matrix composites and analyze the effectiveness of such bimodal microstructures for strengthening composites consisting of a pure Al matrix reinforced with Fe3Al particles. Preferential microstructural refinement limited to the surface of the particles, where the Fe3Al phase is progressively fragmented, occurs during ball milling of the Al-Fe3Al composite powder mixtures. The refined surface becomes the continuous fine-grained matrix that encloses macro-regions with coarser reinforcing particles in the harmonic composites synthesized during subsequent powder consolidation. The generation of the bimodal microstructure has a significant influence on the strength of the harmonic composites, which exceeds that of the conventional material by a factor of 2 while retaining considerable plastic deformation. Finally, modeling of the mechanical properties indicates that the strength of the harmonic composites can be accurately described by taking into account both the volume fraction of reinforcement and the characteristic microstructural features describing the harmonic structure.