The dataset provided here is intended for publication - Harmonized and Open Energy Dataset for Modeling a Highly Renewable Brazilian Power System. The assembled dataset comprises the following subcategories as detailed in the Method section of the publication: i) map of the defined region, ii) aggregated grid network topology, iii) vRES potentials – profile and installable generation capacity, iv) geographically installable capacity of biomass thermal plants, v) hydropower plants inflow, vi) existing and planned power generators with their capacity, vii) electricity load profile, viii) scenarios of sectoral energy demand and iv) cross-border electricity exchanges. This dataset is resolved geographically by Brazilian federal states, and time series data are resolved by hours, spanning the period 2012-2020. The dataset can be used as input to popular open energy system models such as PyPSA and any other modeling framework.