<p>Distinct membraneless organelles within cells collaborate closely to organize crucial functions. However, biosynthetic communicating membraneless organelles have yet to be created. Here we report a binary population of membraneless compartments capable of coexistence, biological communication and controllable feedback under cellular environmental conditions. The compartment consortia emerge from two orthogonally phase-separating proteins in a cell-free expression system. Their appearance can be programmed in time and order for on-demand delivery of molecules. In particular, the consortia can sense, process and deliver functional protein cargo in response to a protease message or a DNA message that encodes the protease. Such DNA-based molecular programs can be further harnessed by installing a feedback loop that controls the information flow at the messenger RNA level. These results contribute to understanding crosstalk among membraneless organelles and provide a design principle that can guide construction of functional compartment consortia.</p><p></p>