The emerging nitrogen-embedded multiple resonance (MR) emitters with an indolo[3,2,1-jk] carbazole (ICz) unit have exhibited promising performance for high-resolution organic light-emitting diode (OLED) devices, while the underlying photophysics has been rarely reported. In this work, the optical spectra, color purity, and emitting efficiency of ICz-based MR emitters were investigated by using electronic structure and thermal vibration correlation function (TVCF) calculations. Unlike B-N MR emitters, the high color purity of investigated ICz-based MR emitters was mainly contributed by considerable structural rigidity, which also greatly affects the radiative decay rate and fluorescence quantum yield of the S1 state. For the majority of investigated emitters, potential reverse intersystem crossing (RISC) channels (T1 → S1 and T2 → S1) are limited by thermally inaccessible ΔEST* or insufficient spin-orbital coupling (SOC), which can be distinguished by the calculated temperature-dependent RISC rate pattern. We provided a systematic photophysical picture for ICz-based MR emitters that might be interesting for the OLED design and application community.