Using organic serniconductor-Containing supramolecule, this study investigates how the small molecule (SM) phase behavior as well as the loading rate and size of the NPs can affect their coassembly in supramolecular frameworks containing strongly interacting molecules. The NPs can be incorporated into the supramolecular microdomains even from a macrophase-separated state. However, the assembly of nanocomposites based on strongly interacting SMs is found to be distinct from both supramolecular nanocomposites based on simple alkyls and supramolecules based on strongly interacting SMs without NPs. The strong crystallization of the SMs tends to force the NPs into less crystalline domains of the comb block, where the SMs are less abundant. The larger NPs favor assembly in the center of the comb domains, parallel to the BCP lamellar axis, to minimize the entropic penalty ofideforming the polymer chain) while the smaller particles assemble into rows in between the comb lamellae, perpendicular to the axis of the BCP lamellae. These studies present a versatile method for the coassembly of strongly interacting, functional SMs with NPs for the fabrication of nanocomposite devices.