An unexpected presence of ferromagnetic (FM) ordering in nanostructured ZnO has been reported previously. Recently, from our detailed magnetization studies and ab initio calculations, we attributed this FM ordering in nanostructured ZnO to the presence of surface states, and a direct correlation between the magnetic properties and crystallinity of ZnO was observed. In this study, through a systematic sample preparation of both pristine and Co-doped ZnO nanostructures, and detailed magnetization and nonlinear optical (NLO) measurements, we confirm that the observed FM ordering is due to the presence of surface states.