This study aimed to assess levels of selected physico-chemical and bacteriological loads of Kalundu stream and Kalundu dam. Sampling was conducted from February to April 2019 in three selected sampling sites. Surface water samples were collected and analyzed for fifteen physico-chemical parameters. Water temperature, pH, turbidity and electrical conductivity were measured on site. Biological oxygen demand (BOD), Chemical Oxygen Demand (COD), total hardness and alkalinity, selected major anions and cations were analyzed at a Water Resources Authority laboratory using standard procedures. Data analysis was carried out using one-way analysis of variance and significant differences accepted at p≤0.05. Results showed that pH, fluoride, sulphates, total hardness and alkalinity were within WHO set standards for drinking water. However, turbidity, EC, Fe, Ca, Mg, Nitrites and Chlorides were above the WHO recommended levels for drinking water. Both total coliforms and E. coli were exceedingly high and ranged from 385±188.9 to 337,133±124,970 MPN/100ml and 70.70±46.50 to 3941183±2771080 MPN/100ml respectively. The findings revealed that water quality of Kalundu stream and Kalundu dam is highly polluted with pathogenic microorganisms and a potential risk to human health. Therefore, measures to curb microbial pollution should be taken by the relevant municipality authorities of Kitui County government.