“…Nonlinear optical (NLO) materials play a pivotal role in various optical applications, such as optical limiting, optical switching, optical communications, and so on. 1–3 A wide range of materials has captured significant attention, including graphene, 4–6 transition metal sulfides, 7–13 black phosphorus, 14,15 perovskite, 16–18 polymers, 19,20 and MXene, 21–26 among others. Within these NLO materials, metal–organic frameworks (MOFs), 27–29 boasting tunable structures and diverse compositions, have emerged as ideal materials for NLO applications.…”