In this paper, we present results from the detailed investigations on the synthesis, optical, emission, electrochemical, and ultrafast nonlinear optical (NLO) properties along with the excited state dynamics of zinc(II) 2,10,16,24-tetrakis(9-phenyl-9H-carbazol-2-yl)phthalocyanine (CBZPC1) and zinc(II) 2,10,16,24-tetrakis(4-(9H-carbazol-9-yl)phenyl)phthalocyanine (CBZPC2). Due to the presence of carbazole moieties, the Soret band was found to be broadened. The emission studies performed using different solvents revealed the fluorescence yields in the range of 0.10-0.27 and the time-resolved fluorescence data revealed radiative lifetimes of, typically, a few nanoseconds. Femtosecond transient absorption measurements indicated the formation of triplet states within the first nanosecond of photoexcitation. From the cyclic voltametric studies, the oxidation and reduction processes were found to be ring centered. Spectral changes in the UV-visible absorption were recorded by means of spectro-electrochemical analysis at an applied potential. The DFT and TD-DFT analysis was employed using B3LYP hybrid functional theory and 6-31G(d,p) basis set in the Gaussian 09 package. The NLO properties of CBZPC1 and CBZPC2 were investigated using the Z-scan technique and femtosecond (fs) pulses with kHz and MHz repetition rates. Closed and open aperture Z-scan data were recorded at three different wavelengths of 600, 700, and 800 nm, and the NLO coefficients were extracted from both types of data. Two-photon absorption (TPA) was the dominant mechanism observed in the open aperture Z-scan data. The real and imaginary parts of the χ(3) along with the two-photon absorption cross sections were evaluated. Our NLO data and large 2PA coefficients and cross sections obtained indicate the potential of these compounds for applications in optical limiting and optical switching applications. © 2019 American Chemical Society.