In this work, the influence of the synthesis parameters (concentration, temperature, and reaction time) on the electrochemical performance of potassium-cobalt(II) octacyanomolybdate (KCoOCM) as a cathode material for its application in lithium-ion batteries was studied. The compound was synthesized hydrothermally using a chemometric approach and characterized by different techniques (FESEM, XRD, TGA). The KCoOCM showed a change in its morphology from prismatic structures to nanorods according to the synthesis conditions. Additionally, there was an influence on the specific capacity as a function of the synthesis parameters, i.e., precursor’s concentrations, temperature, and reaction time. The capacity values reached by the material was 50 mAh g⁻¹, which is close to the theoretical value of the KCoOCM (60 mAh g⁻¹). The statistical method employed would allow finding a condition where it is possible to maximize the capacity value of the material, which has been scarcely studied in this area. Finally, the performance of a lithium-ion battery based on a cathode of KCoOCM is reported for the first time in literature.