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The optimum working conditions of 11 working fluids under different heat source temperatures for an organic Rankine cycle (ORC) were located in our previous work. In the current work, the system irreversibility of each candidate were calculated and compared at their optimal operating conditions. Obvious variation trends of both the cycle efficiency and irreversibility were found for different types of organic fluids. It is suggested, when selecting working fluid for our ORC system, the critical temperature should be as close as possible to the heat source temperature to achieve high cycle efficiency but avoid large irreversibility. The relationships between the structure of the molecules and the critical temperature of the working fluids are investigated qualitatively and potentially meaningful for the rational selection of proper organic fluids for certain ORCs.