A general Ostwald ripening process combined with colloidal soft-matter self-assembly has been developed for coaxing the solid nanoparticle rods into the tubular mesocrystals: self-assembled ZnO microtubules with surface grafting of nanorods, in which the polyelectrolyte is exploited to tailor the forces between the colloidal ZnO nanoparticles and manipulate nanoparticle self-assembly. The strategy presented here can readily be extended to other soft-matter chemical systems that afford colloidal processing.