Heterocyclic organic nonlinear optical materials of N-(1,3-benzothiazol-2-yl)benzamide [2-BTBA] and N-(1,3-benzothiazol-2-yl)-2-fluorobenzamide [2-BTFBA] were orchestrated by benzoylation of 2-aminobenzothiazole utilizing subbed benzoyl chloride. The orchestrated mixtures2-BTBA and 2-BTFBA molecular ion peaks at 253.9 & 272 were affirmed by GC-MS. The grown single crystals of 2-BTBA and 2-BTFBA were developed by slow evaporation method at room temperature with a combination of ethyl acetate & methanol as dissolvable. The X-ray diffraction investigations of equally 2-BTBA & 2-BTFBA crystal have a monoclinic framework with space group P21/n individually. The FT-IR spectra of 2-BTBA and 2-BTFBA show absorption peaks at 1670 and 1660 cm-1, indicating the presence of carbonyl functional group vibration modes in the molecules. UV–Vis spectra show a awesome absorbance band at 303 & 300 nm for 2-BTBA and 2-BTFBA molecules, respectively. The number of protons and carbons were predicted using 1H and 13C NMR spectrum studies. TGA and DTA analyses confirmed the various stages of disintegration of the produced crystals, and they are thermally stable up to 403 K and 333 K for 2-BTBA and 2-BTFBA, respectively. The zone of hindrance method was used to test the antibacterial and antifungal activities of produced single crystals using amphotericin-B and ciprofloxacin as standards. The outcomesprove that the incorporated mixtures display prevalent anti-fungal and antibacterial activity. The non-linear efficiency was affirmed by Kurtz- Perry concentrates trategy for 2-BTBA and 2-BTFBA crystals with the SHG proficiency 2.28 and 2.83 times more prominent than that of potassium dihydrogen phosphate [KDP].