The removal of hazardous heavy metals that have been released into the environment due to industrial activities has become an important issue in recent years. The presented study concerned the removal of copper(II) ions from aqueous solutions using dolomites. Dolomite is a very attractive adsorbent due to its wide availability, low cost, good adsorption, and environmental compatibility. The paper describes the properties of D-I and D-II dolomites from two different open-cast mines in Poland. The properties of natural adsorbents were determined based on point of zero charges (PZC), elemental analysis of the adsorbent composition, FT-IR, XRD, and SEM spectra analysis. Depending on the initial concentration of the solution used, the adsorption efficiency of copper(II) ions was 58–80% for D-I and 80–97% for D-II. The adsorption mechanism in the case of D-II dolomite was mainly based on ion exchange, while chemisorption dominated the D-I dolomite surface. Considering the possibility of the regeneration and reuse of the adsorbent, dolomite D-II is a better material (the desorption efficiency of copper(II) ions was 58–80%). The adsorption behavior of dolomites has been described using six adsorption isotherms. The best fit was obtained for the Redlich–Peterson, Jovanović, and Langmuir isotherms, indicating that monolayer adsorption occurred. The maximum adsorption capacity for copper(II) was 378 mg/g of D-I and 308 mg/g of D-II.