The invention relates to an alterant for ball milling cast iron, in particular to the composite alterant for the nickel aluminum molybdenum-silicon iron alloy loaded nano-aluminum-silicon oxide ball milling cast iron and a preparation method thereof. The alterant is prepared from the following raw materials, by weight, of 2-3 parts of nano-alumina, 1-2 parts of potassium fluoborate, 2-3 parts of nickel powder, 1-2 parts of aluminum powder, 1-2 parts of molybdenum powder, 0.2-0.4 part of oxidized graphene, 1-2 parts of nano silica, 3-5 parts of expanded graphite powder, 1-2 parts of monazite micro powder, 4-5 parts of ferrosilicon powder with the silicon content being 45%, 0.3-0.4 part of magnesium aluminosilicate, 20-25 parts of ethanol aqueous solutions with the concentration being 5%-10% and 0.4-0.5 part of an addition agent. Nano composite powder bodies and a nickel aluminum molybdenum-silicon iron alloy which are loaded by expanded graphite powder are bonded and loaded mutually to prepare the composite alterant with stable performance. The alterant is stable in high temperature, the nucleating effect is good, and graphite spheroidization is stable and durable. According to the alterant, the graphitizing process is facilitated, the structural organization is improved, strength and abrasion resisting are further improved, and compared with a traditional alterant, using is more convenient and faster, and the additional production cost is reduced.