The alternate deposition of exponentially and linearly growing polyelectrolyte multilayers leads to the formation of multicompartment films. In this study, a new system consisting in nanometer-sized multilayer barriers deposited on or between multilayer compartments was designed to respond to mechanical stimuli and to act as nanovalves. The diffusion of polyelectrolytes through the barrier from one compartment to another can be switched on/off by tuning the mechanical stretching and thereby opening or closing nanopores in the barrier. This work represents a first step toward the design of chemically or biologically active films responding to mechanical stresses.