Evidence from epidemiological studies suggests that chronic arsenic exposure may be associated with a higher incidence of hypertension in the population. However, the effect of arsenic exposure on blood pressure remains unexplored in different populations, regions, and regarding arsenic biomarkers. This study investigated 233 arsenicosis patients and 84 participants from a non-arsenic-exposed area to explore the relationship between arsenic exposure and blood pressure and the occurrence of hypertension and wide pulse pressure (WPP) in patients with coal-burning arsenicosis. The results show that arsenic exposure is related to an increased incidence of hypertension and WPP in the arsenicosis population, primarily due to an induced increase in systolic blood pressure (SBP) and pulse pressure (PP) (OR= 1.47, 1.65, allp <0.05). The dose–effect relationships between monomethylated arsenicals (MMA), trivalent arsenic (As3+), hypertension, and WWP were characterized following trend analyses (allp-trend < 0.05) in the coal-burning arsenicosis population. After adjusting for age, gender, body mass index (BMI), smoking, and alcohol usage, compared with low-level exposure, the high level of MMA exposure increases the risk of hypertension by 1.99 times (CI: 1.04–3.80) and the WPP by 2.42 times (CI: 1.23–4.72). Similarly, the high level of As3+exposure increases the hypertension risk by 3.68 times (CI: 1.86–7.30) and the WPP by 3.84 times (CI: 1.93–7.64). Together, the results revealed that urinary MMA and As3+levels are mainly associated with increased SBP and induce a higher incidence of hypertension and WPP. This study provides preliminary population evidence that cardiovascular-related adverse events such as hypertension and WPP ought to be noticed in the coal-burning arsenicosis population.