A peptide nucleic acid(PNA)-peptide conjugated molecule, T′_3(AKAE)_2, was designed to have both a PNA segment for oligonucleotide binding and an ionic self-complementary peptide sequence for self-association. T′_3(AKAE)_2 could co-assemble with oligoadenines(d(A)_x) to form virus-like supramolecular structures whose morphology showed dependence on the chain length and rigidity of the d(A)_x molecules. Smaller nanospheres with diameters of 13.0±2.0 nm were produced in the case of d(A)_6. Wormlike aggregates with lengths of 20–50 nm and diameters of 15.0±2.5 nm were found in the cases of d(A)_(12), d(A)_(18), d(A)_(24) and d(A)_(30). And larger spherical aggregates with diameters of 18±5 nm came into presence in the cases of d(A)_(36) and d(A)_(42). These nanostructures were suggested to be formed under a cooperative effect of base pair recognition and peptidic association. The study provides insights into the programmed assembly of a multi-components system as well as control of the size and shape of the co-assembled structures, which is of great significance in developing gene/drug delivery systems. A peptide nucleic acid (PNA) -peptide conjugated molecule, T’_3 (AKAE) _2 was designed to have both a PNA segment for oligonucleotide binding and an ionic self-complementary peptide sequence for self-association. T’_3 (AKAE) _2 could co-assemble with oligoadenines (d (A) _x) to form virus-like supramolecular structures whose morphology showed dependence dependence of the chain length and rigidity on the d (A) _x molecules. Smaller nanospheres with diameters of 13.0 ± 2.0 nm were produced in the case of d (A) _6. Wormlike aggregates with lengths of 20-50 nm and diameters of 15.0 ± 2.5 nm were found in the cases of d (A) _ (12), d (A) d (A) _ (24) and d (A) _ (30). And larger spherical aggregates with diameters of 18 ± 5 nm came into presence in the cases of d (A) The nanostructures were suggested to be formed under a cooperative effect of base pair recognition and peptidic association. The study provides insights into the programmed assembly of a multi-components system as well as control of the size and shape of the co-assembled structures, which is of great significance in developing gene / drug delivery systems.