The optical and nonlinear optical (NLO) properties of pure boron nitride (BN) cage and super salt (OLi3NO3) doped BN complexes were investigated in this research work utilizing the rB3LYP/6-31G(d,p) density functional theory (DFT) approach. The response mechanism is examined through geometric parameters, frontier molecular orbital (FMO), hyperpolarizabilities, dipole moments (μ), the density of states (DOS), and natural bonding orbital (NBO). Non-covalent interactions (NCl), and infrared spectroscopic (IR) study have been performed to evaluate the nature of interactions and vibrational frequencies of all complexes. As compared to the pure BN surface, the electron transport characteristics of doped complexes were significantly improved when bandgap energies Eg lowered from 6.84 eV to 5.33 eV. The [email protected] demonstrates a considerable increase in the linear polarizability (α0) (248.56 au), and first hyperpolarizability (β0) (553.87 au), because of lower excitations energies as compared to the BN surface (α0=143.01, and β0=29.49). The designed complex [email protected] demonstrated the outstanding NLO properties and observed to be beneficial for constructing future NLO materials.