The world's energy requirement is rising continuously due to an increase in the global population and demand for better quality of life. Fossil fuels are non-renewable, and their consumption poses global warming. Biomass-derived fuels are sustainable alternatives to fossil fuels as they are originated from renewable feedstocks. The present study investigates the production of biocrude from hydrothermal liquefaction of Canadian agricultural straws at identical conditions. Further, barley straw is found to be promising; therefore, hydrothermal liquefaction process parameters are varied for barley straw to maximize the biocrude yield with lower oxygen content. At optimum reaction conditions, the existence of carboxylic acids, phenols, aldehydes, and ketones is identified in the produced biocrude. Further, the recyclability study of the aqueous phase is attempted to explore the possibility of reusing this phase. The physicochemical characteristics of the biocrude (main product) and by-products (hydrochar, non-condensable gases, and aqueous phase) are also studied to identify the suitable areas of applications. The present experimental study demonstrates a detailed understanding of the liquefaction behavior of Canadian barley straw for biocrude production with an immense potential to co-refine in the existing petroleum refineries.