Embedded 3D bioprinting has great value for the freeform fabrication of living matter. However, embedded 3D bioprinting is currently limited to highly viscous liquid baths or liquid‐like solid baths. In contrast, prior to crosslinking, most hydrogels are formulated as low‐viscosity solutions and are therefore not directly compatible with bioprinting due to low shape fidelity and poor print stability. The authors here present a method to enable low‐viscosity ink 3D (LoV3D) bioprinting, based on aqueous two‐phase stabilization of the ink‐bath interface. LoV3D allows for the printing of living constructs at high extrusion speeds (up to 1.8 m s−1) with high viability due to its exceedingly low‐viscosity. Moreover, LoV3D liquid/liquid interfaces offer unique advantages for fusing printed structures, creating intricate vasculature, and modifying surfaces at higher efficiencies than traditional systems. Furthermore, the low interfacial tension of LoV3D bioprinting offers unprecedented nozzle‐independent control over filament diameter via large‐dimension strand‐thinning, which allows for the printing of an exceptionally wide range of diameters down to the width of a single cell. Overall, LoV3D bioprinting is a unique all‐aqueous approach with broad material compatibility without the need for rheological ink adaption, which opens new avenues of application in cell patterning, drug screening, engineered meat, and organ fabrication.