The van der Waals dispersion coefficients of a set of polycyclic aromatic hydrocarbons, ranging in size from the single-cycle benzene to circumovalene (C(66)H(20)), are calculated with a real-time propagation approach to time-dependent density functional theory (TDDFT). In the nonretarded regime, the Casimir-Polder integral is employed to obtain C(6), once the dynamic polarizabilities have been computed at imaginary frequencies with TDDFT. On the other hand, the numerical coefficient that characterizes the fully retarded regime is obtained from the static polarizabilities. This ab initio strategy has favorable scaling with the size of the system--as demonstrated by the size of the reported molecules--and can be easily extended to obtain higher order van der Waals coefficients.