Groundwater contamination in urban cities is imminent in the phase of increased anthropogenic activities apart from the contribution of geogenic contaminants. This study examined the sanitary surveys and hydrochemistry of groundwater in Ado-Ekiti and Ijero-Ekiti to establish the contaminants’ sources, decipher the effects of urbanization on population and explain any relationship between the surveys and the groundwater chemistry. Sanitary surveys of 30 randomly selected wells each from Ado-Ekiti and Ijero-Ekiti were executed by administering and processing appropriately designed questionnaires that addressed salient problems of hygiene and sanitation. The results of the surveys were grouped into very high risk, high risk, intermediate risk, and low risk classes. Subsequently, at each location, in situ parameters (temperature (°C), pH and EC (μS/cm)) were measured using a portable Multi-parameter TestrTM 35 Series S/N: 1382654. At each well, water samples were collected into clean polyethylene bottles in triplicates for cation, anions and e-coli evaluations, respectively. Water samples for cations were acidified by adding two drops of concentrated nitric acid. All samples were kept in a refrigerator at a low temperature of about 4°C before being taken to the Federal University of Technology, Akure, for analyses. Ion chromatography was employed for the anions analysis while the cations were determined using an Atomic Absorption Spectrophotometer Buck 210 model. Membrane filter technique was employed for the e-coli estimation. From the results of the hydrochemistry, the Nitrate Pollution Index (NPI) and Modified Nitrate Pollution Index (MNPI) were estimated and classified into; clean unpolluted, light pollution, moderate pollution, significant pollution, very significant pollution waters. Sanitary surveys in the two cities showed that in the very low risk, intermediate and high-risk categories, Ado-Ekiti had 33.33%, 56.67% and 10% representations, while Ijero-Ekiti had 50%, 23.33% and 26.67% representations, respectively. This observation showed that Ado-Ekiti with higher population and humans’ activities compared to Ijero-Ekiti was less susceptible to pollution. Urbanization has no direct effects on sanitary surveys. The pH of wells’ water in Ado-Ekiti ranged from 4.8 - 8.2, EC (μS/cm) from 101 - 1008, while at Ijero-Ekiti, the pH and EC (μS/cm) varied from 2.1 - 13.8 and 80 - 1008 respectively. Ado-Ekiti wells’ water was more acidic than that of Ijero-Ekiti. Chemical concentrations (mg/L) of Ca2+, Mg2+, Na+, K+, , and Clˉ of the wells’ water in both cities were within WHO-approved standards for drinking water. However, with average concentrations of 142.17 (mg/L) and 252.71 (mg/L) at Ado-Ekiti and Ijero-Ekiti, respectively, exceeded the standard in many locations. Susceptibility to pollution classification employing TDS, NPI and MNPI showed that Ijero-Ekiti was more susceptible to pollution compared to Ado-Ekiti. This assertion was supported by statistical analysis employing correlation, cluster analysis, and principal component analysis. This study showed that urbanization had no direct effects on sanitary surveys and groundwater quality. Pollution of wells’ water in the two cities was, mainly from anthropogenic activities. However, Ijero-Ekiti, with significant anthropogenic activities, had its wells’ water more susceptible to pollution. Sanitary surveys are a complementary method to water quality monitoring.