Drinking water quality is an essential measure of quality of life. This study examined a comparative analysis of the physical and chemical quality of surface and rainwater in Lau Metropolis, Taraba state, by identifying factors responsible for physical and chemical qualities and suggesting a better water body source for domestic use and health well-being. The study was carried out in September 2022, using a purposive sampling technique. Statistical data analysis of Pearson correlation and Chi-square test of mean values were used. The parameters analyzed were pH, Temperature, Electrical conductivity, Turbidity, Colour, and Total Alkalinity. Total Hardness, TDS, Cd, Fe, Zn, Cu and Pb. Laboratory test methods used were ASTM and APHA. The result showed that Harvested Rainwater met specification in all tested parameters except Fe with a concentration of 0.625mg/l as against NSDWQ and WHO's specification of 0.30mg/l. However, Surface water did not meet NSDWQ and WHO specifications in Turbidity, Colour, Fe, and Cd with values of 32.7NTU, 15.17TCU, 0.814mg/l, and 0.013mg/l respectively. The maximum permissible limit by NSDWQ and WHO for Turbidity, Colour, and Cd are 5.0NTU, 15.0TCU, and 0.003mg/l respectively. High Fe content in both water samples could be attributed to contact with dissolved gases from biomass burning, transportation sources, and crustal materials. Land use activities, erosive ability of soil, and stormwater runoff could be responsible for surface water pollution. This study recommends that HRW should be used due to its quality. However, Fe content in HRW can removed domestically by Fe removal filters, it requires less effort and resources. Surface water treatment is expensive