Mountain regions, including Mount Fako and Mount Manengouba, are vital natural water catchments that supply freshwater to over half of the world’s population. These areas play a critical role in delivering potable water through ecosystem services. Although water from the source is typically pure, its quality and quantity decline as it flows downstream, especially through human settlements, resulting in unreliable and intermittent water supply. This study assessed the spatial and seasonal dynamics of water quality in three streams from each mountain—Wolikakwo, Koke, and Ndongo (Mount Cameroon), and Shut, Chambre Noir, and Poladam (Mount Manengouba). Samples were collected at three points along each stream (source, upstream settlement, and downstream settlement) during both dry and rainy seasons. Ten parameters were analyzed using the Weighted Arithmetic Water Quality Index (WQI), with laboratory results compared to WHO drinking water standards. ANOVA and Independent Sample Tests were employed to detect spatial and temporal variations. Findings revealed significant spatial and/or seasonal variations in several streams. In Mount Manengouba, streams showed variations in pH, K⁺, and coliform counts. Chambre Noir and Poladam exhibited significant seasonal changes in conductivity, calcium, sulfates, bicarbonates, and nitrates. In Mount Cameroon, streams like Wolikakwo, Koke, and Ndongo displayed similar patterns, particularly for EC, TDS, temperature, coliforms, and key ions. Overall, WQI results indicated that none of the water sources met WHO standards for potable use. To ensure sustainable water delivery, the study recommends establishing watershed management boards and enforcing water catchment protection laws to safeguard mountain water sources.