The high availability of fluoride in surface and groundwater in the East African Rift Valley was documented during the colonial period. Since the early 1960s, many studies have been conducted to solve the fluorosis crisis in this region. At present, no cost-effective solution to mitigate fluoride contamination is available for the large majority of the population. This situation prompted a process analysis of commonly used technologies. Results revealed that the geochemistry of fluoride is the main problem. Fluoride is very difficult to remove from the aqueous phase. Thus, eliminating the need for technical water defluoridation is an excellent way out of the fluorosis crisis. This goal can be achieved by harvesting fluoride-free rainwater. Harvested rainwater can be mixed with naturally polluted waters in calculated proportions to obtain safe drinking water (blending). This paper presents a concept to transform the Kilimanjaro Mountains into a huge rainwater harvesting park for drinking water supply for the whole East African Rift Valley. However, blended water may contain other pollutants including pathogens that are easy to treat using low-cost methods such as metallic iron based-filters (Fe0 filters). The proposed concept is transferable to other parts of the world still enduring fluoride pollution.