The　precise　control　of　individual　components　in　multicomponent　nanostructures　is　crucial　to　realizing　their　fascinating　functionalities　for　applications　in　electronics,　energy-conversion　devices,　and　biotechnologies.　However,　this　control　remains　particularly　challenging　for　bulk,　multicomponent　nanomaterials　because　the　desired　structures　of　the　constitute　components　often　conflict.　Herein,　a　strategy　is　reported　for　simultaneously　controlling　the　structural　properties　of　the　constituent　components　in　bulk　multicomponent　nanostructures　through　layered　structural　design.　The　power　of　this　approach　is　illustrated　by　generating　the　desired　structures　of　each　constituent　in　a　bulk　multicomponent　nanomaterial　(SmCo　+　FeCo)/NdFeB,　which　cannot　be　attained　with　existing　methods.　The　resulting　nanostructure　exhibits　a　record　high　energy　density　(31　MGOe)　for　this　class　of　bulk　nanocomposites　composed　of　both　hard　and　soft　magnetic　materials,　with　the　soft　magnetic　fraction　exceeding　20　wt%.　It　is　anticipated　that　other　properties　beyond　magnetism,　such　as　the　thermoelectric　and　mechanical　properties,　can　also　be　tuned　by　engineering　such　layered　architectures.