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Internally-cooled dehumidifiers are efficient liquid desiccant dehumidifiers, whose performance is mainly determined by the device structure and operating conditions. Based on energy and mass conservation in the air, solution, and cooling water in the device, mathematical models are built and their theoretical performance is simulated and analyzed in this paper. A novel measure of dehumidification efficiency is introduced to evaluate the performance of internally-cooled dehumidifiers, in which the equilibrium humidity ratio of the inlet solution is calculated according to the minimum temperature in the inlet solution and the cooling water. Numerical simulations show that a counter flow between air and solution is always the most efficient, followed by cross flow, and parallel flow is the least efficient. Cooling water with the same flow direction as the solution performs better than that with a counter flow, with approximately a 5% improvement in efficiency. Compared with CaCl2, the dehumidification efficiency of a LiCl solution is greater by 60%, while its exergy efficiency is less by 16%. Dehumidification efficiency can be improved with the number of air-solution heat transfer units (NTUa-s) increasing, and reduced with the air mass flow rate raised. With NTUa-sincreasing, exergy efficiency can be improved, and an increase in mass flow rate of cooling water results in a decrease of efficiency. Higher solution concentration and lower inlet temperature of solution and air can achieve both higher dehumidification efficiency and exergy efficiency.