Short-wavelength nonlinear optical (NLO) crystals can convert a specific wavelength of light to ultraviolet (UV) and deep-UV region. To date, most of the commercialized UV and deep-UV NLO materials are borate crystals. Borosilicates combine the merits of borates and silicates, they show some unique advantages of rich structural types, moderate second harmonic generation (SHG) response, and high UV transmittance. This paper summarizes the known NLO borosilicates, according to the linkage modes of B-O and Si-O units, these borosilicates can be grouped into two types: (1) borosilicates with B-O-Si covalent bond, and (2) borosilicates with isolated B–O and Si–O units. We discuss the structural features, SHG intensities, and UV cutoff edges of these borosilicates. Future perspectives in this field are given in the final.