A production process for lithium-silicate-based compound is characterized in that: a lithium-silicate compound is reacted with a transition-metal-element-containing substance including iron and/or manganese at from 300° C. or more to 600° C. or less within a molten salt including at least one member being selected from the group consisting of alkali-metal salts under a mixed-gas atmosphere including carbon dioxide and a reducing gas; wherein said transition-metal-element-containing substance includes a deposit that is formed by alkalifying a transition-metal-containing aqueous solution including a compound that includes iron and/or manganese. In accordance with the present production process, lithium-silicate-based compounds including silicon excessively are obtainable. In accordance with the present invention, it is possible to produce materials, which have better battery characteristics than do conventional ones, by means of relatively easy means, regarding lithium-silicate-based materials that are useful as a positive-electrode material for secondary battery.