Here we report on the flattening of water droplets using an ultrathin membrane of autopolymerized polydopamine at the air/water interface. This has only been previously reported with the use of synthetic or extracted peptides, two-dimensional designed synthetic peptide thin films with thicknesses of several tens of nanometers. However, in the previous study, the shape of the water droplet was changed irreversibly and the phenomenon was observed only at the air/water interface. In the present study, an ultrathin polydopamine membrane-stabilized droplet induced the flattening of a water droplet at the air/liquid and liquid/liquid interfaces because a polydopamine membrane was spontaneously formed at these interfaces. Furthermore, a reversible transformation of the droplet to flat and dome shape droplets were discovered at the liquid/liquid interface. These are a completely new system because the polydopamine membrane is dynamically synthesized at the interface and the formation speed of the polydopamine membrane overcomes the flattening time scale. These results will provide new insight into physical control of the interfacial shapes of droplets.