This study was attempted to study for recovery of Li as Li2CO3 from cathode active material, especially NCA (LiNiCoAlO2), recovered from spent lithium ion batteries. This consists of two major processes, carbonation using CO2 and water leaching. Carbonation using CO2 was performed at 600ºC, 700ºC and 800ºC, and NCA (LiNiCoAlO2) was phase-separated into Li2CO3, NiO and CoO. The water leaching process using the differences in solubility was performed to obtain the optimum conditions by using the washing time and the ratio of the sample to the distilled water as variables. As a result, NCA (LiNiCoAlO2) was phase-separated into Li2CO3 and NiO, CoO at 700ºC, and Li2CO3 in water was recovered through vacuum filtration after 1 hour at a 1:30 weight ratio of the powder and distilled water. Finally, Li2CO3 containing Li of more than 98 wt.% was recovered.