High-pressure science has been advancing rapidly in the past several decades due to its potential to access bond engineering and lattice reconstruction. Thanks to the development of pressure devices and advanced in-situ probing technics, it is possible to probe structural phase transitions as well as materials’ optical, electrical, and magnetic properties under extreme pressure, which will in turn help explain new emerging materials’ phases and phenomena. As one of the most popular high-pressure devices, the diamond anvil cell has been used to control the crystal structure and interatomic spacing of materials by applying high pressure while accessing their material properties in-situ. In this dissertation, advanced spectroscopy techniques combined with diamond anvil cells are used to help determine how emergent quantum materials behave under high pressure. A comprehensive summary is offered on the synthesis, characterization, and high-pressure studies of various low-dimensional material systems, such as 2D Ruddlesden-Popper hybrid lead bromide perovskites (CH3(CH2)3NH3)2(CH3NH3)nPbnBr3n+1, (n = 1 and n = 2); guanidinium based lead iodides (2D Gua2PbI4 and 1D GuaPbI3), in which researchers discovered extraordinary luminescent properties and extremely high quantum conversion efficiency; 2D Janus MoSSe and WSSe monolayers, in which the mirror symmetry is broken and an electrical field is built in due to different electronegativity of the top and bottom atom layers; and 2D tellurene, which possess a large potential application in optoelectronic devices and sensors. In combination with the density function theory simulations of such collaborators as Dr. Can Ataca (organic–inorganic halide perovskite), Dr. Arunima K. Singh (tellurene), and Dr. Houlong Zhuang (Janus), this study offers comprehensive and detailed insights into the fundamental physics and mechanics of how crystal structure and band structure evolve at high pressure, discovering new phases, understanding the phase transition mechanism, and determining optoelectronic device applications.