A new ground electronic state potential energy surface of Li⁺ + N₂ system is presented in the Jacobi scattering coordinates at MRCI level of accuracy employing the augmented correlation-consistent polarized valence quadrupole zeta (aug-cc-pVQZ) basis set. An analytic fit of the computed ab initio surface has also been obtained. The surface has a global minimum for the collinear geometry at the internuclear distance of N₂, r = 2.078a₀, and the distance between Li⁺ and N₂, R = 4.96a₀. Quantum dynamics studieshave been performed within the vibrational close coupling-rotational infinite-order sudden approximation at E_c.m = 3.64 eV, and the collision attributes have been analyzed. The computed total differential crosssections are found in quantitative agreement with those available from the experiments at E_c.m = 3.64 eV. The other dynamic attributes such as angle dependent opacities and integral cross-sections are also reported.Preliminary rigid-rotor and vibrational–rotational coupled-state calculations at Ec.m.= 2.47 eV also support the experimental observation that the system exhibits a large number of rotational excitations in the vibrational manifold v = 0