Background: We described the prevalence of cardiovascular risk factors in groups of Brazilian Indigenous people at different degrees of urbanization. Methods: The Project of Atherosclerosis among Indigenous populations (Projeto de Aterosclerose em Indígenas; PAI) is a cross-sectional study conducted in Northeast Brazil between August 2016–June 2017. It included three populations: Fulni-ô Indigenous people (lowest degree of urbanization), Truká Indigenous people (greater urbanization), and a highly urbanized non-Indigenous local cohort (control group). Participants were assessed to register sociodemographic, anthropometric, as well as clinical and laboratory-derived cardiovascular (CV) risk parameters. Age-adjusted prevalence of hypertension was also computed. Nonparametric tests were used for group comparisons. Results: Here we included 999 participants, with a predominance of females in all three groups (68.3% Control group, 65.0% Fulni-ô indigenous group, and 60.1% Truká indigenous group). Obesity was present in 45.6% of the urban non-Indigenous population, 37.7% Truká and in 27.6% Fulni-ô participants. The prevalence of hypertension was 29.1% (n = 297) with lower prevalence in the less urbanized Fulni-ô people (Fulni-ô – 18.2%; Truká – 33.9%; and Control – 33.8%; p < 0.001). In the elderly male population, the prevalence of hypertension was 18.7% in the Fulni-ô, 45.8% in the Truká, and 54.5% in the control group. Of the 342 participants that self-reported hypertension, 37.5% (n = 68) showed uncontrolled blood pressure (BP). Uncontrolled BP was more prevalent among Truká people when compared to Fulni-ô people and non-Indigenous participants (45.4%, 22.9%, and 40.7%, respectively; p < 0.001). Conclusions: We found a higher cardiovascular risk in communities with a higher degree of urbanization, suggesting that living in towns and cities may have a negative impact on these aspects of cardiovascular health.