Currently, interest to lithium and lithium-ion all-solid-state power sources is rapidly growing all over the world. However, several issues should be addressed before all-solid-state batteries production: high resistance values of the solid electrolyte membrane and poor contact between electrolyte and electrode materials. The transition to thin-film technologies is one of the promising ways to solve these problems. Tape casting can be proposed to obtain thin-film solid electrolytes. In this research, the features of the structure formation, morphology and lithium-ion conductivity of Li7La3Zr2O12 films were investigated. Li7La3Zr2O12 films with the thickness of 35 μm were obtained by tape casting on Ni substrate. The influence of organic components content on homogeneous coatings formation was established. Heat treatment conditions for dried films were chosen based on differential scanning calorimetry and optical dilatometry. Phase change from tetragonal to cubic modification occurs after annealing the Li7La3Zr2O12 films at 700 °C and higher. The annealed Li7La3Zr2O12 films have developed surface, which can lead to improved contact between the solid electrolyte and an electrode in an electrochemical cell. Li7La3Zr2O12 films annealed at 800 °C have the highest lithium-ion conductivity values (2.5 10 7 and 1.5 10 5 S cm 1 at 90 and 215 °C, respectively). The technology of Li7La3Zr2O12 films formation with the thickness of ~23 μm by tape casting was developed.