The quality of the machined surface and reduced carbon footprint are crucial factors for the operational effectiveness and lifetime of the manufactured components. Direct energy deposition (DED) can be employed to create large and complex metal parts, but low-dimensional accuracy usually requires finishing by a subtractive process. The present work deals with the sustainability assessment and machinability analysis in the machining of laser-melted titanium-based composites (TiC–Ti64-ELI) for the aviation sector. In this regard, the milling experiments were performed under distinct environmentally friendly cooling conditions. The results were analyzed in terms of environmental concerns, such as carbon emissions and specific cutting energy, as well as machining quality characteristics, including surface roughness and tool wear. The results indicate that cryogenic cooling with the carbon dioxide (Cryo-CO2) technique with laser-melted titanium composites can significantly lower carbon emissions while maintaining high-quality performance standards required in aviation applications. The desirability function was employed to obtain the best speed-feed combinations and environmental conditions for milling TiC–Ti64-ELI. The derived optimal conditions are Vc = 60 m/min, fr = 0.082 mm/rev, and Cryo-CO2 cooling. In addition, sustainable assessment was employed to study the effectiveness of environmental conditions.