Large variations in fluoride concentrations exist in natural waters, many of which are the source of community drinking-water supplies. Determining fluoride concentrations in community drinking waters can be challenging in developing Pacific countries such as Vanuatu that have limited laboratory capacity. Knowledge of naturally elevated fluoride concentrations that cause irreversible, adverse health outcomes may allow communities the opportunity to treat and manage their drinking-water supplies. Community drinking-water samples (n = 69), sourced from groundwaters, roof catchment rainwaters, surface waters and springs, were sampled on Tanna Island, Vanuatu between 2017 and 2020. In an 18 km² area of Western Tanna, a set of 30 groundwater-based drinking-water samples had a median fluoride concentration of 3.3 mg/L, with 20 samples >1.5 mg/L and seven samples >4.0 mg/L. These concentrations increase the risk of dental and skeletal fluorosis, respectively. Repeat resampling at five sites showed little variation over the sampling period. Rainwater-fed drinking-water supplies were lower overall and highly variable in fluoride concentrations (<0.05–4.0 mg/L, median of 0.53 mg/L), with variable inputs from volcanic emissions from Yasur volcano. We recommend a comprehensive oral health and bone health study for the whole island to determine adverse health effects of excess fluoride in this vulnerable population.