The miniaturization of magnetic sensors and storage devices down to the nano-scale leads to drastic changes in magnetic phenomena compared with the same devices with a larger size. Excited-nuclear-probe (radioactive probe) techniques are ideal for investigating these new magnetic nanostructures. By observing the magnetic hyperfine fields (and in some cases the electric-field-gradients (EFGs)) at the nuclei of radioactive probes, microscopic information about the magnetic environment of the probes is acquired. The magnetic hyperfine field is particularly sensitive to the s-spin polarization of the conduction electrons and to the orbital magnetic moment of the probe atom. Three methods of inserting radioactive probes into magnetic nanostructures are presented; neutron activation, recoil implantation and 'soft-landing', followed by descriptions of their application to selected examples. In some cases, these methods offer the simultaneous creation and observation of new magnetic materials at the atomic scale. This review focuses firstly on the induced magnetism in noble-metal spacer layers between either ferromagnetic (FM) or FM/antiferromagnetic (AFM) layers in a trilayer structure. Using the method of low-temperature nuclear orientation, the s-spin polarization of noble-metal probes was measured and was found to be very sensitive to the magnetic properties at both the FM and AFM interfaces. Secondly, the recoil implantation of radioactive Fe probes into rare-earth hosts and d-band alloys and subsequent measurement using time-differential perturbed angular distribution offer the possibility of controlling the chemical composition and number of nearest-neighbours. This method was used to prepare local 3d-magnetic clusters in a non-magnetic matrix and to observe their magnetic behaviour. Finally, non-magnetic radioactive probes were 'soft-landed' onto Ni surfaces and extremely lattice-expanded ultrathin Ni films. By measuring the magnetic hyperfine fields and EFGs at 111 Cd probes using time-differential perturbed angular correlation (TDPAC), it was possible to distinguish the interaction of Cd probes located at various surface This article was invited by Professor S Washburn.