Five D-pi-A-A type of heterocyclic polycyclic aromatic hydrocarbons (hetero-PAHs) organic molecules with quinacridone (QA) derivatives as the core bridge connected with different donor groups of triarylamine (T), indoline derivative (W), and carbazole (K) and the auxiliary acceptor groups benzobisthiadiazole (B) and furan (F) have been designed. The potential application of designed sensitizers in solar cells and photocatalysis have been investigated. Microscopic major processes involve dye regeneration, electrons recombination, intramolecular charge transfer (ICT) properties and key parameters of molecular photoelectric performance. Besides, the coupling strength, energy gaps, dipole moments, molecular fluorescent lifetime and the bonding type between dye and TiO2 were estimated to reveal the nature of photocatalysis. Results indicated that introducing W or B unit should improve the photoelectric performance among all design strategies (especially, simultaneously introducing two moieties) due to the excellent electron-donating ability of W and the pull electrons' ability of B auxiliary acceptor. Designing WQAB@TiO2 and WQAF@TiO2 to have better photocatalytic properties owing to the stronger interaction and surface charge transfer, particularly for WQAB. Current molecular strategies using controlling moieties provide a choice for potential applications in solar cells and photocatalytic fields.