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Microwave-assisted pyrolysis of Chlorella vulgariswas carried out under compound additives, which contained catalyst (ZSM-5) and microwave absorbent (graphite). The effects of three independent variables (Si/Al ratio of ZSM-5, additives amount and catalyst ratio) on the weight loss characteristics, product yield and energy consumption were investigated. Response Surface Methodology (RSM) coupled with Box-Behnken Design (BBD) was used to optimize pyrolysis time (Ts) and bio-oil yield (Bo) of Chlorella vulgarispyrolysis under three independent variables. The results showed that compound additives can promoted the pyrolysis progress and increased the bio-oil yield. Besides, compound additives can also reduce the energy consumption of bio-oil production in most cases. The predicted results showed that optimal Tsand Bowere 3550s and 22.70%, respectively. GC-MS analysis further revealed that compound additive has stronger effect on denitrogenating than single additive, which is of great significance in alleviating nitrogen oxide pollution caused by bio-oil with high nitrogen content.