A versatile strategy to ameliorate the lack of structural integrity of low-viscosity inks for extrusionbased 3D bioprinting by inclusion of complex-forming block polyelectrolyte additives. Rapid, charge-driven self-assembly into a protective hydrogel scaffolding (micelles or interconnected networks) provides enhanced shear and tensile properties to the bioink and enables continuous extrusion at 37 °C without the need of chemical crosslinking between individual layers. This approach hence paves the way for fast biomanufacturing of human-scale tissue constructs with improved inter-layer bonding.