Aqueous two-phase systems (ATPS) have a great potential in many biotechnological applications. ATPS are highly sensitive to shear forces due to their low interfacial tension. In this work, we investigated an ATPS composed of gelatin methacrylate (GelMA) and dextran and studied the influence of shear on the microstructure of hydrogels that were obtained by crosslinking the GelMA phase. To study the influence of an applied shear on the microstructure of the resulting hydrogel, we employed a two-step approach based on UV-rheology by applying a constant shear followed by the photocrosslinking in situ of the GelMA phase to quench the shear-induced structures. The resulting hydrogels were analyzed by confocal laser scanning microscopy. Two main systems based on a single GelMA concentration and two dextran concentrations were investigated. In the absence of shear, these latter results followed the crosslinking of the GelMA phase in either porous GelMA or bicontinuous hydrogels at pH 4.9. Anisotropic hydrogels with highly aligned strings or hydrogels with aligned porous band channels are formed as a function of the applied shear at pH 4.9. Next, we demonstrated how fine-tuning the pH affected the shear-induced microstructures. A decrease in the pH resulted in the transition of the bicontinuous system, from string with a thin fibers structure to well-defined fibers and then to larger microfilaments with aggregated GelMA particles. A further decrease of the pH near the GelMA isoelectric point led to the formation of a multiple emulsion of Dextran/GelMA/Dextran. The shear of such a system at a shear rate of 100 s⁻¹, followed by photocrosslinking of the GelMA phase, resulted in the formation of porous GelMA particles coexisting with blocks of GelMA porous hydrogel. The diversity of the formed microstructures and the particular interest in using GelMA highlight their potential for developing functional soft materials for many biotechnological applications.