“…Nonlinear optical (NLO) materials play a pivotal role in various optical applications, such as optical limiting, optical switching, optical communications, and so on. [1][2][3] A wide range of materials has captured significant attention, including graphene, [4][5][6] transition metal sulfides, [7][8][9][10][11][12][13] black phosphorus, 14,15 perovskite, [16][17][18] polymers, 19,20 and MXene, [21][22][23][24][25][26] among others. Within these NLO materials, metal-organic frameworks (MOFs), [27][28][29] boasting tunable structures and diverse compositions, have emerged as ideal materials for NLO applications.…”