The interest in helix-containing nanostructures is currently growing as a consequence of their potential applications in areas such as nanomedicine, nanomaterial design, chiral recognition, and asymmetric catalysis. Herein, we present a facile and tunable one-pot methodology to achieve chiral nano-objects. The nickel-catalyzed coordination polymerization-induced self-assembly (NiCCo-PISA) of helical poly(aryl isocyanide) amphiphilic diblock copolymers was realized and allowed access to various nano-object morphologies (spheres, worm-like micelles, and polymersomes). The helicity of the core block was confirmed via circular dichroism (CD) spectroscopy for all morphologies, proving their chiral nature. Small-molecule uptake by the spherical nanoparticles was investigated by encapsulating Nile Red into the core of the spheres and subsequent transfer into aqueous media. The presence of a CD signal for the otherwise CD-inactive dye proved the chiral induction effect of the nano-objects' helical core. This demonstrates the potential of NiCCo-PISA to prepare nanoparticles for applications in nanomaterials, catalysis, and recognition.