One of the main concerns of this work was to find out how the reaction conditions affect the microstructure and homogeneity of the ACNs. Using the MQ experiment described in the experimental section, we analyzed samples synthesized under different conditions (CN1-1 to CN9-3) in terms of their connectivities (see Scheme 1), isotropic (defect) fractions, and related average RDCs. We refrain from discussing the results of the sample series CN1 to CN3 in detail, which were dried after gelation and were subject to post-curing (see Figure ). However, the connectivities of these samples are summarized in the SI (see Table ).