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A heat pump driven atmospheric water harvesting system, which can be operated under direct cooling mode and desiccant wheels assisted cooling mode, was proposed in this paper. Investigations were carried out to find out the optimal operation mode and operation parameters under different ambient conditions and daily water harvesting requirements. Optimization studies were firstly carried out on each operation mode to find the recommended operation parameters, namely evaporation temperature and daily operation hours, for different ambient conditions, daily water harvesting rate and maximum operating hours. Then, the optimal operation modes, which has lower daily power consumption under their own recommended operation parameters, were suggested on the psychrometric chart. The results showed that, for different combinations of daily water harvesting rate and maximum operating hours, there exist a critical humidity ratio and a critical relative humidity ratio for each case. When ambient air relative humidity and humidity are both higher than the critical values, it is recommended to use the direct cooling mode. Otherwise, the desiccant wheels assisted cooling mode should be used. Lastly, performances of the system in different climate zones were analyzed. Under the optimal operation mode, the annual average water harvesting efficiency was from 1.08 to 1.22 kg/kWh in Urumqi, from 1.50 to 1.78 kg/kWh in Beijing, and from 2.22 to 3.72 kg/kWh in Haikou, respectively, when daily water harvesting rate is from 50 to 200 kg/day and maximum operating hours is from 6 to 10 h. • Propose a water harvesting system that can be operated under two operating modes. • Study the optimized operating parameters and performances for each operating mode. • Suggest optimal mode based on ambient conditions and water harvesting requirements. • Study annual performances in three typical cities with different climate conditions. [ABSTRACT FROM AUTHOR]