Rayon is an extremely valuable cellulosic fiber in the global textile industry. Since cuprammonium rayon is more eco-friendly than other types of rayon fabrics, it was synthesized by regenerating α–cellulose isolated from wastepaper using a novel gaseous-ammoniation injection (GAI) process. This was achieved by preparing tetra–ammine copper hydroxide (cuoxam solution) via reacting copper sulfate and sodium hydroxide to produce copper hydroxide that was, finally, ammoniated by injecting the gas directly to the reaction vessel instead of using ammonium hydroxide applied by prior art. After that, the air-dried cellulose was chemically generated by dissolving it in a freshly prepared cuoxam solution and, subsequently, was regenerated by extruding it within a hardening bath constituted mainly from citric acid, producing the cuprammonium rayon (c. rayon). The properties of the fibrous, structural (XRD and mechanical), physical, and chemical features were investigated. It was found that the rayon was produced in a high yield (90.3%) with accepted properties. The fibrous properties of the rayon staple length, linear density, and fiber diameter were found to be 44 mm, 235 Tex, and 19.4 µm, respectively. In addition, the mechanical properties determined, namely tensile strength, elongation at break, modulus of elasticity, and breaking tenacity, were found to be 218.3 MPa, 14.3 GPa, 16.1%, and 27.53 cN/Tex, respectively. Based on this finding, and upon injecting the ammonia gas through the α–cellulose saturated and immersed in the Cu (OH)2 to complete producing the cuoxam solvent, we find that theuse of an injection rate of 120 mL/minute to obtain the highest fibers’ tensile strength for the final product of the c. rayon is preferable. Utilization of higher rates will consume more amounts of the ammonia gas without gaining noticeable enhancement in the c. rayon’s mechanical quality. Accordingly, the GAI invention rendered the c. rayon favorable for use in making sustainable semisynthetic floss for either insulation purposes or spun threads for woven and nonwoven textile clothing.