Furthermore, the versatile use of bPE additives enabled a simple transfer to other liquid-like materials. In another proof-of-principle experiment, we employed DbPEs to render norborneneand thiol-functionalized gelatin (GelNB/GelS) as well as poly(ethylene glycol) diacrylate (PEGDA) extrudable at 37 °C. We note that different inks will require material-specific demands for bPE loadings to reach appropriate viscoelastic properties for extrusion. This printability optimization was pursued only for GelMA inks. In the following, we will limit our study to the GelMA/bPE system and discuss the benchmarks for printable formulations in bioink design using small amplitude oscillatory shear (SAOS) rheology. We also evaluate the impact of the additives on material properties and highlight the utility and the potential of self-assembling bPEs in 3D bioprinting. (A) 5 wt% GelMA precursor solution supplemented with 20 wt% oppositely charged DbPEs that form a protective hydrogel scaffolding to enable continuous extrusion of a hollow square structure (11 layers) at 37 °C, followed by a single photocrosslinking step in the end. Shape fidelity of structures printed with the hybrid ink is significantly improved as compared to the print results of bPE-free GelMA inks which rely solely on thermally induced gelation by a cooled cartridge and print bed and hence suffer from loss of structural integrity with increasing layer stacking. (B) Extrusion of multiple layers of a grid without photocrosslinking between individual layers using a 5/20 wt% GelMA/DbPE formulation. Pore integrity of the grid was preserved for the first 18 layers. (C) Transfer of the bPE additive-based approach to other low-viscosity inks (semi-synthetic and synthetic) exemplified by extrusion of a 5 wt% GelNB/GelS and PEGDA precursor solution supplemented with 20 wt% and 40 wt% DbPEs, respectively (scale bar: 1 cm).