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The enhancement of polymer properties via molecular composites formulation attracts increased attention from both the scientific and the industrial communities. Molecular composites are intimate blends where the rigid-rod polymer molecularly reinforced the flexible matrix. The primary factor restricting the composite materials creation is phase separation due to the incompatibility of the rigid-rod molecule and flexible polymer matrix. The one approach to the phase separation elimination is preparation of graft copolymers with rigid polymer backbones and flexible thermoplastic side chains or block copolymers containing rigid and flexible blocks. Previously [1] we have reported about significant improvement of polycaproamide performance properties by in situ anionic polymerization of ε-caprolactam in the presence of aromatic polyimides. A unique feature of polyimides is that depending on the formation parameters they play the role of polyfunctional activator in anionic polymerization of ε-caprolactam due to its own imide cycles. However unsufficient polyimide solubility in the molten ε-caprolactam restricts of their application. In this research, we present our first results on the fabrication of new molecular composites based on polycaproamide and polyamideimides as activators. Polyimide blocks in such activators reduce the formation of covalent bonds between polymer matrix and polyimide backbone as well as polyamide blocks increase the solubility. All obtained composites were thoroughly examined by various techniques including thermogravimetric and elemental analysis, TMA, mechanical tests, etc. It was shown thermal stability, Izod impact strength of polymer blocks have been significantly improved.