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In this work, a series of isotactic-polypropylene/atactic-polystyrene (<i>i</i>PP/<i>a</i>PS) miktoarm star copolymers, P_xS_y, was synthesized via an arm-first approach. Varied star macromolecule architectures were fabricated by designing the arm length and the arm numbers (x and y). These miktoarm stars were able to form micelles in selective solvent (<i>N</i>,<i>N&#8242;</i>-dimethylformamide (DMF)), in which the insoluble <i>i</i>PP arms formed the core and the soluble <i>a</i>PS arms formed the shell. The miktoarm polymers aggregated to micro-nanoscale binary structures (MNBSes) in the casting process, and their morphologies, including the MNBS shape and size, were greatly influenced by the P_xS_y architectures. The MNBSes endowed the material surface with superhydrophobic performance with a water contact angle of 157.0&#176; and a sliding angle of 1.5&#176;.