The effect of initial salt composition on the formation of zero-valent bimetallic FeCo was investigated in this work. Pure crystalline zero-valent FeCo nanoparticles (NPs) were obtained using either chloride or nitrate salts of both metals. Smaller NPs can be obtained using nitrate salts. Comparing the features of the FeCo prepared at room temperature and the solvothermal method revealed that both materials are almost identical. However, the room-temperature method is simpler, quicker, and saves energy. Energy-dispersive X-ray (EDX) analysis of the FeCo NPs prepared using nitrate salts at room temperature demonstrated the absence of oxygen and the presence and uniform distribution of Fe and Co within the structure with the atomic ratio very close to the initially planned one. The particles were sphere-like with a mean particle size of 7 nm, saturation magnetization of 173.32 emu/g, and surface area of 30 m2/g. The removal of Cu2+ and reactive blue 5 (RB5) by FeCo in a single-component system was conformed to the pseudo-first-order and pseudo-second-order models, respectively. The isotherm study confirmed the ability of FeCo for the simultaneous removal of Cu2+ and RB5 with more selectivity toward Cu2+. The RB5 has a synergistic effect on Cu2+ removal, while Cu2+ has an antagonistic effect on RB5 removal.