In this study, two different green microalgae, Chlamydomonas nivalis (C. nivalis) and Nannochloropsis gaditana (N. gaditana), were cultivated in open ponds and the harvested wet biomass was converted to bio-crude by hydrothermal liquefaction (HTL) with/without catalyst. Catalytic HTL experiments were performed by using copper-exchanged zeolites including Cu-MOR, Cu-ZSM-5, and Cu-SSZ13, synthesized by recently developed supercritical ion exchange method using scCO2. The composition of all bio-crudes was analyzed by elemental analysis and GC/MS. First, the effects of different operating conditions on the yields of the products and the bio-crude composition were determined for non-catalytic process. Temperature, duration, and water/algae biomass ratio in the feed were the process parameters investigated in the ranges of 250–350 ºC, 10–60 min, and 5–20 wt%, respectively. For C. nivalis, 300 ºC, 60 min, and water/algae ratio of 4 were the optimum conditions which led to maximum bio-crude yield of 18.8 wt%, while 300 ºC, 30 min, and water/algae ratio of 9 were the optimum ones for N. gaditana at which the maximum bio-crude yield of 34.0 wt% was observed. Bio-crude yield of N. gaditana was improved using Cu-MOR, while using catalysts for the case of C. nivalis resulted in more gasification with no positive effect on bio-crude yield. Moreover, elemental analysis showed that the fraction of nitrogen and oxygen in biocrude decreased in catalytic HTL runs, in line with the GC/MS results showing that the concentration of hydrocarbons and cyclic compounds increased in the presence of catalysts accompanied by a decrease in concentration of nitrogenous compounds.