Abstract: Antiferromagnetic materials are receiving renewed interest on behalf of their potential for information technologies. Recent reports have also revealed how the physics governing such magnetic arrangements and their excitations become more complex compared to traditional ferromagnetic materials, especially at the nanoscale. Here, we address two main issues that are of prime interest to their technological transfer. First, using small-angle neutron scattering, we show the existence of a magnetic helix-like super-structure in a polycrystalline TbCu2 alloy, preserved at both bulk and nanoparticle ensembles of 8 nm. Second, using inelastic neutron scattering, we elucidate the magnetic excitons and the crystalline electric field energy level schemes of TbCu2 in bulk and nanoparticle ensembles. This allows to understad the effect of the surface broken symmetry on the quantum energy levels at the nanoscale, so as the key role of interfacial effects on the propagation of magnetic excitations. Our research provides insights for the realization of magnetic moment dynamics models based on complex nanometric super-structures, and for nanoparticles to be integrated in spintronics and information technology applications.