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The high overpotentials for oxygen reduction reaction (ORR) create an extremely negative impact on the energy efficiency of the air-based battery systems. To overcome this problem, binuclear ball-type metallophthalocyanines containing methoxy substituents (M₂Pc₂(EP)₄, M = Fe(II), Co(II) and Zn(II)) were wrapped with polystyrene sodium sulfonate (PSS) modified graphene oxide (GO), using a facilely “solvothermal π-π assembly” method to prepare M₂Pc₂(EP)₄/PSS-Gr composites. Compared with the commercial Pt/C catalysts, the M₂Pc₂(EP)₄/PSS-Gr composites enhanced the catalytic activity of oxygen reduction reaction. The π electron conjugated structure of the MN₄-type phthalocyanine macrocyclic system strongly influenced the one-step four-electron electrocatalytic process of the M₂Pc₂(EP)₄/PSS-Gr composites. Moreover, the π-π interactions between the M₂Pc₂(EP)₄ and PSS-Gr dramatically enhanced the π electron density in the conjugated structure and oxygen could be reduced more easily. The electrocatalytic activity test was displayed in the order of Fe₂Pc₂(FP)₄/PSS-Gr > Co₂Pc₂(EP)₄/PSS-Gr > Zn₂Pc₂(EP)₄/PSS-Gr. The results indicated that the catalytic performance of M₂Pc₂R_n could be enhanced by the modification of π electron conjugated structure of M₂Pc₂(EP)₄ and carbon materials.