Our approach, based on electrostatic self-assembly, hence excelled by enabling fast and smooth fabrication with only a single crosslinking step in the end and by its versatile use for all types of liquid-like precursors (Figure ). Moreover, our strategy addressed multiple current shortcomings faced by the temperature-controlled GelMA inks, particularly long holding times in the cartridge for cooling promoting cell sedimentation and imposing unnecessary thermal stress on the cells, discontinuous fabrication accompanied by stacking of disjointed layers, and inefficient temperature transfer from the print bed to the top layers of the deposited ink in larger constructs. Last but not least, the bPE-triggered gain of remarkably increased viscosity at 37 °C is not only relevant for extrusion-based bioprinting but is also of great interest for biomedical injections in order to prevent fast diffusion from the injection site prior to secondary crosslinking.