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In this work, we propose a strategy to design new deep‐ultraviolet (deep‐UV) nonlinear optical (NLO) materials through the combination of borate and phosphate NLO material genome. Accordingly, a series of borophosphates are predicted with very large energy bandgaps, strong second harmonic generation (SHG) effects, and moderate birefringence in the deep‐UV region. In particular, two novel fluoride borophosphates, PBO3F2 and PB3O6F2, are able to achieve the deep‐UV SHG laser output with shorter phase‐matching wavelengths (≈155 and 137 nm) than that of KBe2BO3F2 (KBBF, ≈161 nm). Further calculations show that these two structures are dynamically and thermodynamically stable, thus triggering possible synthesis, growth, and applications of them. The results attest that the proposed strategy is instructive and pave a comprehensive road map for us to discover new NLO crystals, especially in the borophosphate catalog with excellent deep‐UV phase‐matching capabilities beyond KBBF. [ABSTRACT FROM AUTHOR]

• Single crystal structure of a novel ultraviolet NLO tourmaline was solved. • Sellmeier equations were obtained by fitting the measured refractive indices. • Phase matching range of the title crystal is obtained from the Sellmeier equations. • The linear and NLO properties were investigated by the experimental and theory calculation. Transparent tourmaline NaAl 9 (BO 3) 3 Si 6 O 21 OH is first reported by combining experimental and theory calculation methods, which exhibits potential ultraviolet nonlinear optical properties. [Display omitted] Tourmaline, as an important mineral, has received intensive interest, since it is not only a valuable gemstone, but also is a piezoelectric or pyroelectric material, due to the polar structural configuration. However, its nonlinear optical (NLO) properties were not explored so far, because a transparent crystal with high transmittance is scarce, being essential to optical functional materials. Here, we report a novel ultraviolet (UV) NLO tourmaline crystal with chemical composition NaAl 9 (BO 3) 3 Si 6 O 21 OH for the first time by combining first-principles analysis and experimental measurements. It exhibits a short UV absorption edge, considerable second harmonic generation effect and moderate birefringence, thereby facilitating its phase-matching coherent beam output in the range from visible to UV regions. [ABSTRACT FROM AUTHOR]