Concave microstructures such as microwells and microgrooves are widely utilized in fields such as biochips, microfluidics, and functional devices. Previously, concave microstructure fabrication was mostly based on laser etching or lithography which is either costly or of multisteps. The inkjet etching method is a direct structuring technique, but limited by its inherent transverse ink diffusion that leads to low feature resolution. Nanoimprint lithography can reach submicro and even nano ranges, whereas an elaborate template is needed. Thus, it is still a challenge to realize controllable fabrication of concave microstructures in large areas with high efficiency and resolution. Here, a template‐free strategy to fabricate concave microstructures with high resolution by inkjet imprinting is provided. In this method, a sacrificial ink is inkjet‐printed onto a precured viscoelastic surface and imprints its shapes to construct concave microstructures. The morphology of the microstructures could be adjusted by controlling the interaction between the two immiscible phases. The microwells/microgrooves could be used to pattern single cells and functional materials such as optical, electronic, and magnetic nanoparticles. These results will open a new pathway to fabricate concave microstructures and broaden their applications in various functional devices.