LAUSR

Significance Biomolecular condensates are highly diverse systems spanning not only homogeneous liquid droplets but also gels, glasses, and even multiphase architectures that contain various coexisting liquid-like and/or gel-like inner phases. Multiphase architectures form when the different biomolecular components in a multicomponent condensate establish sufficiently imbalanced intermolecular forces to sustain different coexisting phases. While such a requirement seems, at first glance, impossible to fulfil for a condensate formed exclusively of chemically identical proteins (i.e., single component), our simulations predict conditions under which this may be possible. During condensate aging, a sufficiently large imbalance in intermolecular interactions can emerge intrinsically from the accumulation of protein structural transitions—driving even single-component condensates into nonequilibrium liquid-core/gel-shell or gel-core/liquid-shell multiphase architectures.