“…The field of nonlinear optics has witnessed incredible milestones in recent years, with significant strides made in the development of materials showcasing exceptional nonlinear optical properties. , Materials exhibiting nonlinear optical behavior are renowned in advanced technological applications, including photonics, optoelectronics, optical limiting, optical switching, laser technology, and optical computing, etc. − These materials exhibit distinct behaviors, such as frequency conversion, Pockel’s and Kerr electro-optic effects, optical signal modulation, harmonic generation, etc., paramount for various applications. − The remarkable nonlinear optical characteristic arises from the unique interplay of structure−property relationship, delocalization of electron clouds achieved within the molecular systems, diverse interactions such as π-conjugation, charge transfer through metal-to-ligand and ligand-to-metal, hydrogen bonding interactions, etc. ,,, Various intriguing topological features of metal−organic frameworks with diverse molecular structures, high porosity, huge surface area, and postsynthetic modifiability and the flexibility of linkers and metal nodes make MOFs predominantly exquisite candidates for nonlinear optical materials . In the presence of donor−acceptor groups, delocalized π-electrons in azo-dye compounds identify them as promising nonlinear optical stuff .…”