Having established the efficacy of the C22G1 self-assembled dendrimers for coagulation control in terms of high-affinity, multivalent electrostatically-driven heparin binding and pharmaceutically-useful degradation, and disassembly profile, we decided to investigate the impact of amphiphilic dendron structural modifications on their self-assembled morphology and the related polyanion binding effect. Computer-assisted design based on multiscale molecular simulations ultimately yielded the two dendritic cationic compounds (C12)2-L-Asp-L-Lys and (C12)2-L-Asp-L-Lys-(L-Lys)2 (hereafter called L-G1 and L-G2, Figure 6a,b), which were predicted to self-assemble into worm-like cylindrical and spherical micelles, respectively (Figure 6b,c) [26,38].