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Bronze-steel bimetallic structures are structural components finding a growing application in industrial sectors such as aerospace, power generation, and machinery. Recent legislation on green economy and sustainable manufacturing is boosting industry to implement innovative manufacturing processes and new metal alloys capable of lowering environmental footprint by avoiding toxic substances. Laser Metal Deposition is a cost-effective Additive Manufacturing technique for producing bimetallic components by limiting material waste and reducing energy consumption. In this research work, the influence of the main LMD process parameters on the final quality of CuSn11Bi3 coatings on C45 surfaces is analyzed. The Cu-based powder is specifically designed and developed to reduce environmental pollution and increase worker safety by avoiding the use of hazardous chemical elements. The performed observations demonstrate that high-density (99.90%) and crack-free clads are feasible by preventing melt pool dilution zones. Cu diffusion into the C45 substrate deteriorates the structural integrity at the clad-substrate interface by inducing liquid metal embrittlement cracking, whereas steel diffusion into the as-deposited clad promotes crack propagation. High-density (up to 99.97%) and crack-free CuSn11Bi3 coatings are achieved by using low specific energies (from 17 J/mm2 to 40 J/mm2) and reducing the Oxygen content during sample manufacturing up to 0.02%.