Cycloparaphenylenes (CPPs) are nanosized structures with challenging isolated and bulk properties. They can be also viewed as synthetic targets for the template-driven (potentially) bottom-up synthesis of carbon nanotubes. Thus, the step by step understanding of the supramolecular order at the nanoscale is of utmost relevance for further molecular engineering. We find here that intra-molecular noncovalent (dispersion) interactions must be taken into account to obtain accurate estimates of structural and optoelectronic properties of these[n]CPP compounds, analyzing also their influence as the number of repeat units increases from n = 4 up to n = 12, both in the gas phase and in solution. We also address the supramolecular self-assembly of