We report in situ low-energy electron diffraction intensity versus voltage [LEED-I(V)] studies of the surface atomic structure of epitaxially grown (001)pc-oriented (pc=pseudocubic) thin films of the correlated 3d transition-metal oxide LaNiO3. Our analysis indicates the presence of large out-of-plane bucklings of the topmost LaO layers but only minor bucklings of the topmost NiO2 layers, in close agreement with earlier surface x-ray diffraction data. In view of materials design approaches that have suggested using atomic-scale polar structural distortions to produce designer electronic structures in artificial nickelate heterostructures, we propose that the broken inversion symmetry inherent to the surface of rare-earth nickelate thin films offers a similar opportunity to study the coupling between atomic structure and electronic properties in this family of materials. © 2017 American Physical Society.