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Aluminoborates (ABOs) show wide ultraviolet (UV) transmittance, and are one of the important types of UV and deep-UV nonlinear optical (NLO) materials. In recent years, the combination of AlOn (n = 4, 5, 6) polyhedra or their fluorinated analogues with different polyborate anions leads to a rich variety of crystalline ABOs. In this review, we summarize the recent developments of UV and deep-UV NLO inorganic ABOs. These ABOs can be grouped into three types in terms of their compositions: (i) aluminum oxyborates, (ii) alkali/alkaline earth metal aluminoborates, and (iii) alkali/alkaline earth metal aluminoborate fluorides and fluoroaluminoborates. We discuss the synthesis, structural features, NLO properties, as well as related structure-performance relationships of these non-centrosymmetric ABOs. Finally, the future perspectives in this field are discussed.