This study assessed the water quality for drinking and irrigation purposes on the southern slopes of Mt. Kilimanjaro during the dry season under low flow conditions. Fifty-one samples covering eight different water sources (i.e., stream water from natural and anthropogenic impacted streams, domestic water, spring water, rainfall, groundwater, lake water and water from irrigation canals) were collected in a snapshot sampling campaign over 10 days in February 2023. First, physical, chemical and biological parameters were analysed and compared with Tanzanian and international drinking and irrigation water quality requirements. The samples were then ranked according to their suitability for drinking and/or irrigation using water quality indices (WQI). All drinking water quality parameters except for E. coli and turbidity were within the permissible limits. A generalised problem of faecal contamination was found in the study area, including in domestic water, highlighting the need to identify sources of contamination and remediate them before distribution. The drinking water quality index (DWQI) classified 89% of the samples as unsuitable and 11% as excellent for drinking. Irrigation water quality parameters were within the guidelines of restriction of use except for pH in 5 samples. In contrast to the DWQI, the vast majority of the water samples (88%) can be used for irrigation without restrictions according to the irrigation water quality index (IWQI). The suitability of water for irrigation was also assessed using three indices, i.e., Kelley’s Index, Soluble Sodium Percentage and Magnesium Ratio, which indicated potential problems with excess of sodium (about 30% of the samples) and magnesium (about 20%). Further studies combining suitability indices, soil characteristics and crop types are recommended to assess water quality for irrigation use.