A metallophthalocyanine carbon complex is designed by a simple approach to achieve superior, bifunctional catalytic activity. A simple and cost-effective technique is utilized to prepare carbon iron phthalocyanine composites. Furthermore, to investigate ball milling effects, iron phthalocyanine is ball milled, which is used to prepare the carbon ball-milled iron phthalocyanine composites. All the prepared composites exhibit better catalytic activity in both oxygen reduction and oxygen evolution reactions than Pt/C, indicating carbon support significantly improves the stability, conductivity, and surface properties of iron phthalocyanine. The ball-milling improves specific surface area, which in turn enhances the oxygen evolution reaction activity of the composites. When the carbon-iron phthalocyanine composites were applied to an air-cathode catalyst in a lithium-oxygen battery, high reversibility and low over-potential were attained. Among all the synthesized catalysts, the reduced graphene oxide_ball-milled iron phthalocyanine composite exhibits superior bifunctional electrocatalytic activity with high reversibility (92%) and low over-potential (0.7 V) due to enhanced surface properties.