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Arsenic (As) is a highly toxic, carcinogenic trace metal that can potentially contaminate groundwater sources in volcanic regions. This study provides the first comparative documentation of As concentrations in groundwater in a volcano-sedimentary region in the Philippines. Matched, repeated As measurements and physico-chemical analyses were performed in 26 individual wells from 11 municipalities and city in Batangas province from July 2020 to November 2021. Using the electrothermal atomic absorption spectrometric method, analysis of the wells revealed that in 2020, 23 out of 26 (88.46%) had As levels above the WHO limit of >10 ppb while 20 out of 26 wells (76.92%) had persistently high As levels a year later. Using a Wilcoxon signed-rank test, levels of As were found to be statistically elevated compared to the national safe limit of 10 pbb in the 26 matched sampling sites in both 2020 (p-value < 0.001) and 2021 (p-value = 0.013). Additionally, a two-paired Wilcoxon signed-rank test revealed that As levels were statistically higher in 2020 than in 2021 (p-value = 0.003), suggesting that As levels may be higher in years when there is more volcanic activity; however, this remains to be further elucidated with suitable longitudinal data, as this study is still in its preliminary stages. The data was also analyzed using a bivariable regression, which showed no evidence of a significant relationship between As levels and distance from the danger zone (Taal volcano crater); however, results showed an inverse but statistically insignificant relationship between As levels and elevation. Due to the toxic profile and persistence of As in groundwater in Batangas Province, continuous groundwater As monitoring, timely public health risk communication, and the provision of alternative water sources to affected populations are recommended.