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In this paper, we consider an Li-ion battery as a grey system. The grey prediction technique is then used to develop a grey-predicted Li-ion battery charge system (GP-LBCS). The proposed GP-LBCS is designed to replace the general constant-voltage (CV) mode using the GP mode to improve the Li-ion battery charge behavior. A GP algorithm is built in GP-LBCS to make the charge trajectories faster and safer. A 3-D Y-mesh diagram for describing the charge trajectories of the proposed GP-LBCS is simulated. A GP-LBCS prototype is designed and implemented to assess the charge performance. Experiments show that the charge speed and the charge efficiency of the proposed GP-LBCS, compared with the general constant-current-CV charge system, are increased above 23% and 1.6%, respectively. The charge speed and efficiency in the proposed GP mode are improved above 34% and 7%, respectively, compared with that in the general CV mode.