Gelatin methacryloyl (GelMA) is a widely used semi-synthetic polymer for a variety of bioapplications. However, the development of versatile GelMA hydrogels requires tuning of their microstructure. Herein, we report the possibility of preparing hydrogels with various microstructures under shear from an aqueous two-phase system (ATPS) consisting of GelMA and dextran. The influence of an applied preshear on dextran/GelMA droplets and bicontinuous systems is investigated by rheology that allows the application of a constant shear and is immediately followed by in situ UV-curing of the GelMA-rich phase. The microstructure of the resulting hydrogels is examined by confocal laser scanning microscopy (CLSM). The results show that the GelMA string phase and GelMA hydrogels with aligned bands can be formed depending on the concentration of dextran and the applied preshear. The influence of the pH of the ATPS is investigated and demonstrates the formation of multiple emulsions upon decreasing the charge density of GelMA. The preshearing of multiple emulsions, following gelation, leads to the formation of porous GelMA microgels. The diversity of the formed structures highlights the application potential of preshearing ATPS in the development of functional soft materials.