Here, we present a versatile strategy to imbue printability to crosslinkable low-viscosity inks at 37 °C by inclusion of polyelectrolyte complex (PEC) self-assemblies. In the model system demonstrated here, oppositely charged diblock or triblock polyelectrolytes (DbPEs and TbPEs) serve as building blocks of electrostatic self-assemblies -micelles or network, respectively while gelatin methacryloyl (GelMA) at 37 °C serves as a representative low-viscosity photocurable ink. Mixing of the three ink constituents (the oppositely charged block polyelectrolytes and the crosslinkable precursors) results in swift assembly of GelMA-containing viscous and extrudable PEC hydrogel inks. The PEC hydrogels recover quickly (significantly faster than hydrogen-bonded biopolymer hydrogels) upon deposition, providing structural robustness and enabling multi-layer printing. Photocrosslinkability of GelMA chains remains conserved in the PEC hydrogel inks, and UV exposure of the 3D printed manifolds results in an interpenetrating combination of a covalent network and non-covalent electrostatic assemblies. As compared to GelMA manifolds, these photocured interpenetrating network hydrogel manifolds exhibit improvements in shear and tensile properties, including shear and tensile moduli, toughness, and extensibility, as well as provide control over their swelling response. We demonstrate suitable GelMA/DbPE and GelMA/TbPE formulations for 3D bioprinting, as identified by rheological screening, and continuous extrusion of 3D structures which require only a single photocrosslinking step in the end. Proof-of-concept printing demonstrations with diverse photocrosslinkable inks highlight the versatility and transferability of our approach. We envision PEC hydrogels to emerge as powerful additives to any type of liquid-like precursor solution that will expand the future availability of extrusion bioinks for tissue engineering and pave the way for fast biomanufacturing of humanscale tissue constructs with improved inter-layer bonding.