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Abstract The radiation mechanism underlying the prompt emission remains unresolved and can be resolved using a systematic and uniform time-resolved spectro-polarimetric study. In this paper, we investigated the spectral, temporal, and polarimetric characteristics of five bright gamma-ray bursts (GRBs) using archival data from AstroSat CZTI, Swift Burst Alert Telescope, and Fermi/GBM. These bright GRBs were detected by CZTI in its first year of operation, and their average polarization characteristics have been published in Chattopadhyay et al. In the present work, we examined the time-resolved (in 100–600 keV) and energy-resolved polarization measurements of these GRBs with an improved polarimetric technique such as increasing the effective area and bandwidth (by using data from low-gain pixels), using an improved event selection logic to reduce noise in the double events and extend the spectral bandwidth. In addition, we also separately carried out detailed time-resolved spectral analyses of these GRBs using empirical and physical synchrotron models. By these improved time-resolved and energy-resolved spectral and polarimetric studies (not fully coupled spectro-polarimetric fitting), we could pin down the elusive prompt emission mechanism of these GRBs. Our spectro-polarimetric analysis reveals that GRB 160623A, GRB 160703A, and GRB 160821A have Poynting flux-dominated jets. On the other hand, GRB 160325A and GRB 160802A have baryonic-dominated jets with mild magnetization. Furthermore, we observe a rapid change in polarization angle by ∼90° within the main pulse of very bright GRB 160821A, consistent with our previous results. Our study suggests that the jet composition of GRBs may exhibit a wide range of magnetization, which can be revealed by utilizing spectro-polarimetric investigations of the bright GRBs.