Low‐dimensional metal halides (LDMHs) represent a promising class of materials in various luminescent applications because of their self‐trapped exciton (STE) emissions with unique properties such as broad luminescence spectra, large Stokes shift, and high color rendition. LDMHs at the molecular level can be constructed, including 2D layers, 1D chains, and 0D clusters assembled by polyhedra units, all of which exhibit significantly different luminescence properties from 3D MHs. The dimensional regulation of LDMHs has been explored for years, including the choice of organic cations, modulating electron‐phonon coupling effect, and adding external temperature and pressure. Herein, this review discusses the synergy between structural engineering and solvent effects for LDMHs, including the emission mechanisms for LDMHs and the roles solvent molecules play in regulating the dimensions. In addition, challenges and opportunities for LDMHs are discussed to shed light on the future development of novel materials with multifunctional optical properties suitable for practical applications.