Fabrication of nanostructures with great complexity and regularity is a topic of intense current interest because of their importance both in fundamental theories and applications. Here we report an interesting finding of the formation of ordered polymeric double helices with precise structures and high stability. These uniform double helices are hierarchically self-assembling results of undulated multicompartment cylinders which formed from primary amphiphilic mixed-shell nanoparticles. Diblock copolymers of P2VN-b-PAA (poly-(vinylnaphthalene)-block-poly(acrylic acid) and PEO-b-PAA (poly-(ethylene oxide)-block-poly(acrylic acid)) were noncovalently/electrostatically cross-linked into amphiphilic PEO/P2VN-shelled nanoparticles by 1,6-hexyldiamine in a common solvent DMF. When the common solvent changed into selective ones (water), undulated cylinders were facilely obtained due to their hydrophobic interparticles interactions. After a certain time aging, these undulated cylinders self-organized into finally thermodynamic-stable double helices with complex but regular superstructures. The conditions and processes of assembling were carefully examined through extensive experiments.