Nonlinear optical crystalline material is the fascinating tool for the optoelectronic devices and for phase-matched equipments, frequency matching circuits and etc. Present study portrays the synthesize and utility of macro and nano scaled crystals of 2-[4-(trifluoromethyl) phenyl]-1H-benzimidazole (TFMPHB) by slow evaporation solution growth method and by milling conversion. As-prepared crystals were studied by XRD, CHNSO analysis, dielectric and tribology-mechanical, NLO, and photoconductivity. The orthorhombic phase structure with the average crystalline size of 21 nm was observed. The elemental composition of crystals was analyzed for the presence of elements. Tribological studies of macro and nano TFMPHB crystals were favorable for mechanical applications. Further, the high dielectric constant (363 K) at low frequency was suitable for microelectronic devices; NLO is analyzed with phase matching effect over particle size, and photoconductivity study also reported for the entitled crystalline specimen. The structural parameters by AFM and SEM, absorbance nature by UV spectra, and modeling data by computational methods are also reported.