There is increasing concern about the cardiovascular effects of mercury (Hg) exposure, and that organic methylmercury and inorganic Hg2+ may affect the cardiovascular system and blood pressure differentially. In small-scale gold mining communities where inorganic, elemental Hg exposures are high, little is known about the effects of Hg on blood pressure. In 2011, we assessed the relationship between Hg exposure and blood pressure (BP) in a cross-sectional study of adults from a small-scale gold mining community, Kejetia, and subsistence farming community, Gorogo, in Ghana’s Upper East Region. Participants’ resting heart rate and BP were measured, and hair and urine samples were provided to serve as biomarkers of organic and inorganic Hg exposure, respectively. Participants included 70 miners and 26 non-miners from Kejetia and 75 non-miners from Gorogo. Total specific gravity-adjusted urinary and hair Hg was higher among Kejetia miners than Kejetia non-miners and Gorogo participants (median urinary Hg: 5.17, 1.18, and 0.154 µg/L, respectively; hair Hg: 0.945, 0.419, and 0.181 µg/g, respectively). Hypertension was prevalent in 17.7% of Kejetia and 21.3% of Gorogo participants. Urinary and hair Hg were not significantly associated with systolic or diastolic BP for Kejetia or Gorogo participants while adjusting for sex, age, and smoking status. Although our results follow trends seen in other studies, the associations were not of statistical significance. Given the unique study population and high exposures to inorganic Hg, the work contained here will help increase our understanding of the cardiovascular effects of Hg.