A novel semiorganic nonlinear optical (NLO) crystal, bis(thiourea) barium nitrate (BTBN) was synthesized and grown by slow evaporation method. Structure of the new crystalline compound was confirmed by single crystal X-ray diffraction analysis and it showed that BTBN belongs to orthorhombic crystal system. The crystalline nature of the BTBN was confirmed by powder X-ray diffraction study. Important functional groups of BTBN were identified by FT-IR spectroscopic analysis. UV-Vis-NIR spectral study showed that the grown crystal is transparent in the entire visible region with low cut off wavelength of 304 nm. BTBN exhibits a SHG efficiency which is nearly 2.38 times higher than that of KDP. The BTBN crystal has high mechanical strength and belongs to soft category, which was confirmed by micorhardness study. The thermal stability of BTBN was determined from TGA and DTA thermal study which revealed that the BTBN crystal has thermal stability up to 243.1 °C. The surface properties and presence of elements was analyzed by SEM and EDAX study, respectively.