A large photonic band gap (PBG) is highly favorable for photonic crystal devices. One of the most important goals of PBG materials research is identifying structural design strategies for maximizing the gap size. We provide a comprehensive analysis of the PBG properties of two-dimensional (2D) quasicrystals (QCs), where rotational symmetry, dielectric fill factor, and structural morphology were varied systematically in order to identify correlations between structure and PBG width at a given dielectric contrast (13:1, Si:air). The transverse electric (TE) and transverse magnetic (TM) PBGs of 12 types of QCs are investigated (588 structures). We discovered a 12mm QC with a 56.5% TE PBG, the largest reported TE PBG for an aperiodic crystal to date. We also report here a QC morphology comprising “throwing star”-like dielectric domains, with near-circular air cores and interconnecting veins emanating radially around the core. This interesting morphology leads to a complete PBG of ∼20% , which is the largest reported complete PBG for aperiodic crystals.