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The co-liquefaction behaviors of cotton seed (CS) and flos populi (FP) were investigated in the sub-critical water/ethanol mixed solvent using the medical stone (MS) based additives. Oil products were characterized using FTIR, GC-MS, 1HNMR, and 13CNMR techniques. The test results showed that the synergistic effect of co-liquefaction was obvious when the ratio of cotton seed and flospopuli was 1:1 without additives. The additives, such as 12-phosphotungstic acid (PW12), HZSM-5, PW12/HZSM-5 and modified medical stone (MS), PW12/MS, Ni/MS, Co/MS, Mo/MS and Co-Mo/MS, could increase the bio-oil yield; and the modified MS resulted in higher liquefied oil yield than that achieved by MS. Furthermore, additives such as Ni/MS, Mo/MS, and Co-Mo/MS also could increase the yield of aliphatic hydrocarbons in liquefied oil. The addition of Co-Mo/MS could lead to a highest liquefied oil yield of 28.8％, while the additive of PW12/HZSM-5 could result in a highest total conversion of 81.6％. Results also revealed that additives, such as PW12/MS, PW12, PW12/HZSM-5, Ni/MS, Co/MS, Mo/MS, and Co-Mo/MS, could increase the H2 production and decrease the CO2 production in gas products.