Proton-conducting electrochemical devices such as protonic ceramic fuel cells and protonic ceramic electrolysis cells play a major role in the creation of eco-friendly “green” energy systems. The most studies of proton-conducting materials for these devices are barium cerate zirconates. The layered perovskites are novel class of proton-conducting materials. In this paper, the possibility of cation and oxyanion doping of layered perovskite BaNd2In2O7 was carried out for the first time. The most conductive composition BaLa1.9Sr0.1In2O6.95 demonstrates protonic conductivity value 2·10−5 S/cm at 450 °C. The acceptor-doped two-layer perovskites are the prospective class of proton-conducting materials, and further modification of their composition opens up a new way in the design of solid oxide protonic conductors.