The domestic water (DW) quality of an island province in the Philippines that experienced two major mining disasters in the 1990s was assessed and evaluated in 2021 utilizing the heavy metals pollution index (MPI), Nemerow’s pollution index (NPI), and the total carcinogenic risk (TCR) index. The island province sources its DW supply from groundwater (GW), surface water (SW), tap water (TP), and water refilling stations (WRS). This DW supply is used for drinking and cooking by the population. In situ analyses were carried out using an Olympus Vanta X-ray fluorescence spectrometer (XRF) and Accusensing Metals Analysis System (MAS) G1 and the target heavy metals and metalloids (HMM) were arsenic (As), barium (Ba), copper (Cu), iron (Fe), lead (Pb), manganese (Mn), nickel (Ni), and zinc (Zn). The carcinogenic risk was evaluated using the Monte Carlo (MC) method while a machine learning geostatistical interpolation (MLGI) technique was employed to create spatial maps of the metal concentrations and health risk indices. The MPI values calculated at all sampling locations for all water samples indicated a high pollution. Additionally, the NPI values computed at all sampling locations for all DW samples were categorized as “highly polluted”. The results showed that the health quotient indices (HQI) for As and Pb were significantly greater than 1 in all water sources, indicating a probable significant health risk (HR) to the population of the island province. Additionally, As exhibited the highest carcinogenic risk (CR), which was observed in TW samples. This accounted for 89.7% of the total CR observed in TW. Furthermore, all sampling locations exceeded the recommended maximum threshold level of 1.0 × 10−4 by the USEPA. Spatial distribution maps of the contaminant concentrations and health risks provide valuable information to households and guide local government units as well as regional and national agencies in developing strategic interventions to improve DW quality in the island province.