The present work reports on the ultrafast nonlinear optical (NLO) properties of a series of D-π-Α and D-A push-pull carbazole-based dyes and establishes a correlation between these properties and their efficiency for potential photonic and optoelectronic applications, such as multiphoton lithography (MPL). The ultrafast NLO properties of the studied dyes are determined by two distinct experimental techniques, Z-scan and pump-probe optical Kerr effect (OKE), employing 246 fs laser pulses at 515 nm. The results indicate that chemical functionalization of the carbazole moiety with various strong electron-donating and/or electron-withdrawing groups, such as benzene, styrene, 4-bromostyrene, nitrobenzene, trimethyl isocyanurate, methyl, and indane-1,3-dione, can result in a controlled and significant enhancement of the NLO absorptive and refractive responses. In the context of potential applications, the efficiency of carbazole-based organic materials as photoinitiators (PIs) for MPL applications is demonstrated. The fabricated woodpile microstructure using chemically functionalized carbazole as a PI demonstrates improvements in both resolution and MPL efficiency compared to that using unfunctionalized carbazole as a PI. This attributed to efficient charge transfer resulting from chemical functionalization, which leads to a substantial increase (approximately one order of magnitude) in the values of the imaginary part of the second-order hyperpolarizability (Imγ) and the two-photon absorption cross section (σ). The achieved resolution of 280 nm is comparable to that obtained with other widely used PIs in MPL applications. Additionally, owing to strong NLO refraction and Kerr signal of the studied functionalized carbazole, they also exhibit promise as candidates for all-optical switching applications in telecommunications, optical computing, data processing, etc.