Results of studies of the properties of hybrid MF-4SC membranes with a gradient distribution of hydrated zirconia nanoparticles through the thickness prepared by layer-by-layer casting from a polymer solution are described. The effect of the dopant concentration on the properties of the membranes is studied. At a low oxide concentration, the water uptake and ionic conductivity of the resulting samples increase compared to the original MF-4SC membrane. It is found that the diffusion permeability of HCl and NaCl solutions across these membranes exhibits an asymmetric behavior. It is shown that the diffusion permeability is higher in the case of diffusion of the solutions from the unmodified side of the membrane. The maximum asymmetry coefficient is obtained for a membrane containing 10% ZrO2 in the modified layer for the diffusion of 0.1 M HCl solution (38%). The causes of the diffusion permeability asymmetry are discussed.