This study focuses on a countercurrent leaching process (CLP) for the dissolution of high-value metals from cathode active material of spent lithium-ion batteries (LIBs). Its main aim is to improve the effective utilization of acid during leaching and allow for the continuous operation of the entire CLP by adjusting the process parameters. The overall recovery of lithium (Li), cobalt (Co), nickel (Ni), and manganese (Mn) was 98%, 95%, 95%, and 92%, respectively; the acid utilization of the leaching process exceeded 95% under optimum conditions. The optimum conditions for first stage leaching were 70 g/L solid–liquid (S/L) ratio at 40°C for 30 minutes, and 2.0 M sulfuric acid, 100 g/L S/L ratio, 7 g/L starch, at 85°C for 120 minutes for second stage leaching. After five bouts of circulatory leaching, more than 98% Li, 95% Co, 95% Ni, and 92% Mn were leached under the same leaching conditions. Furthermore, we introduced the Avrami equation to describe metal leaching kinetics from spent LIBs, and determined that the second stage leaching process was controlled by the diffusion rate. In this way, Li, Ni, Co, and Mn can be recovered efficiently and the excess acid in the leachate can be reused in this hydrometallurgical process, potentially offering economic and environmental benefits.