The state of copper species stabilized in nanosized LTL zeolite subjected to various post-synthesis treatments was unveiled by a range of spectroscopic techniques. FTIR and UV-Vis studies demonstrated that the reduction process of copper in the LTL nanosized zeolite leads to the formation of different species including Cu2+, Cu+ and Cu nanoparticles (Cu NPs). The adsorption of probe molecules (NO and CO) was used to selectively monitor the copper species in the LTL nanosized zeolite upon oxidation and reduction post-synthesis treatments. Both the Cu2+ and Cu+ species were probed by NO and CO, respectively. The amount of Cu+ in the LTL zeolite nanocrystals was about 43% as determined by FTIR, while the amount of Cu NPs was about 55% determined by the UV-Vis spectroscopic characterization. These results were complemented by EPR, 29Si and 63Cu MAS NMR spectroscopic data. The EPR spectroscopy was further applied to monitor the effective reduction of the Cu2+ species and their re-oxidation, while the 63Cu MAS NMR verified the presence of Cu NPs in the LTL nanosized zeolite crystals.