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An accurate assessment of the harmonious relationship between human beings and water resources is central to conducting the comprehensive management of water resources. The human-water relationship in the “Belt and Road” region is complex, but there is a lack of systematic quantitative research. An inadequate understanding of the human-water relationship hinders decision-makers in recognizing water management priorities. To fill this gap, this paper first selects six criteria for human-water harmony from the perspectives of a humanistic system and a water system. Based on these criteria, representative indexes were selected, and the harmony degree equation was used to calculate the degree of human-water harmony in 43 countries along the “Belt and Road” in 2002, 2007, 2012 and 2017. The results revealed that human-water harmony mainly exhibited a high rate of change in developing countries, while harmony was relatively stable in developed countries and generally higher than that in developing countries. At the same time, countries in the “Belt and Road” region had different human-water relationship problems, and it was necessary to solve these problems according to their national conditions. This study can be used by countries to propel themselves out of their unique situation and understand the human-water relationship from an overall perspective by conducting a comparative analysis of different countries at the national scale. These results can provide a reference for solving the harmonious development problem of the human-water relationship in countries along the “Belt and Road”.