Inspired by earlier findings and conjectures, our study focuses on analyzing the structural deformation and rotational dynamics of both organic and inorganic layers, including the investigation of hydrogen bonding between these layers, with the aim to understand how these factors collectively governs the phase transition process. The phenomena and mechanisms identified in our study provide valuable insights into the design principles for selecting organic and inorganic components in the context of phase transitions, aimed at enhancing the stability and performance of hybrid organic-inorganic layered perovskites at various temperatures.