The synergistic effect of rigid organic framework and soft lattice makes metal‐organic framework (MOF) luminescent materials more widely used. Herein, 2D lead‐MOFs are reported that produce white light through the coregulation of free excitons and self‐trapped excitons. The synthesized BIF‐142‐Cl shows outstanding white‐light emission with the CIE color coordinates of (0.312, 0.335) close to pure white light, the excellent color rendering index (CRI) of 90.4, and the gentle correlation color temperature (CCT) of 5364 K. Meanwhile, the multicolor emission from blue to white light can be adjusted by changing the excitation wavelength. Furthermore, photophysical studies confirm that the strong electronic phonon coupling in the excited state of lead halide polyhedrons is directly responsible for the generation of self‐trapped excitons. This synthetic strategy of introducing tunable dual emission centers not only offers a prospect for the development of solid‐state lighting materials but also widens the path to the fields of anticounterfeiting, display media, and information identification.