consequence of the momentum transfer dependence of the measured magnitudes, providing spatial resolution which can be tuned by choosing the proper probe and/or experimental conditions. In particular, neutron-scattering (NS) techniques provide two additional advantages for soft-matter investigations, such as: i) the possibility to match simultaneously the right length and time scales, and ii) the possibility to label selectively the components of a complex material via deuterium labeling. [2][3][4][5][6][7][8] Illustrative examples of the importance of deuterium labeling in polymeric systems were the pioneering experiments on labeled polymer melts realized in the 1970s [9,10] -as soon as the first small-angle neutron-scattering (SANS) instruments were developed-providing experimental evidence for the random coil conformation of linear macromolecules in bulk, as originally proposed by Flory. [11] Modern single-chain nanoparticles (SCNPs) prepared by intramolecular cross-linking of individual functional polymer chains can be considered as bioinspired soft nano-objects [12][13][14][15][16][17][18][19][20][21][22] with promising prospects for enzyme-mimetic catalysis, [23][24][25][26][27][28][29][30][31][32] nanomedicine [33][34][35][36][37][38][39][40][41] and several other potential applications. [42] Access to full perdeuterated functional polymer precursors to produce completely deuterated single-chain nanoparticles (dSCNPs) for NS is limited by the fact that most of the functional monomers as well as reactive cross-linkers currently in use are not commercially available in their deuterated version. Even with this severe limitation, NS studies with partially deuterated SCNPs have proven: i) the "crumple-globule"-like conformation of SCNPs when embedded in a linear polymeric matrix, [43,44] ii) the SCNP-induced matrix entanglement dilution in a polymer nanocomposite, [45] and iii) the confined dynamics of a low-T g polymer in the matrix of a nanocomposite rich in SCNPs, even at temperatures where the latter are above their T g . [46] However, deploying the full possibilities of the NS techniques for investigating the structure and dynamic features of SCNPs, as model macromolecules to address the effect of chain topology on materials properties, has been constrained by the absence of dSCNP samples. Their availability is a prerequisite for investigations of functions as important as, for example, the single-chain dynamic structure Single-Chain Nanoparticles Access to completely deuterated single-chain nanoparticles (dSCNPs) has remained an unresolved issue. Herein, the first facile and efficient procedure to produce dSCNPs is reported, which comprises: i) the use of commercially available perdeuterated cyclic ether monomers as starting reagents, ii) a ringopening copolymerization process performed in bulk to produce a neat dSCNP precursor, iii) a standard azidation reaction to decorate this precursor with azide moieties, and iv) a facile intramolecular azide photodecomposition step carried out under UV irradiation at...