Motivated by the recent electrode health diagnosis method that requires selective open-circuit voltage data, this paper presents a novel approach for the fast acquisition of battery equilibrium voltage using bidirectional current pulses. The proposed method was found by solving a minimum-time optimal control problem. Unlike the conventional pulse-relaxation method which requires a long relaxation period, the use of charge and discharge pulses reduces the testing time by 69%. The given problem is studied numerically and analytically. Analysis based on Pontryagin's minimum principle (PMP) demonstrates that the solution is either bang–bang or bang–off–bang control, depending on the constraints. Furthermore, the optimal control problem is reformulated into a finite-dimensional switching-time optimization problem, making it computationally tractable for on-board applications. Finally, experimental validation is presented for a 4.5 Ah NMC/graphite cell showing a 73% time reduction to reach a new equilibrium voltage.