Arsenic contamination of groundwater has emerged as a significant challenge for the human right to water in India because of over 80% dependence on groundwater for drinking, particularly in the rural areas. In order to mitigate the arsenic menace and provide safe drinking water to the masses, government and non-governmental agencies have initiated several interventions. These interventions can be categorized under one of the following approaches, namely, treatment of contaminated water; supply of groundwater with acceptable level of arsenic; surface water supply; and rainwater harvesting. While it is a reality that all populations estimated to be ‘at risk’ of arsenic exposure have not yet achieved ‘coverage’ under one or more of these approaches, there exist more pertinent issues. These can be summarized under the rubric of ‘sustainability’ of the interventions, primarily from environmental, social, cultural and economic perspectives. This chapter evaluates the different arsenic mitigation interventions in India from these different sustainability perspectives, and proposes that rainwater harvesting offers the most promising way forward for sustainable arsenic mitigation.