Disclosed is a method of producing high-purity lithium carbonate and barium sulfate from discarded lithium secondary batteries, including: a first process for producing high-purity lithium phosphate from a discarded battery; and a second process for producing lithium sulfate from the lithium phosphate and producing lithium carbonate and barium sulfate from the lithium sulfate. The second process has steps of (a) producing a liquid mixture of lithium phosphate and sulfuric acid, (b) obtaining lithium sulfate by condensing the liquid mixture, (c) dissolving the lithium sulfate in water or a sodium hydroxide aqueous solution, depositing phosphoric acid as lithium phosphate, and performing solid-liquid separation (d) depositing lithium carbonate and performing solid-liquid separation to obtain lithium carbonate, (e) finely grinding the lithium carbonate and classifying the particles, (f) controlling a particle size and shape by dissloving edges of particles or minute particles, (g) performing solid-liquid separation, and (h) depositing barium sulfate.