A facile wet impregnation method was employed to prepare a bimetallic Ni–Cu catalyst on a mesoporous KIT-5 support, keeping the nickel loading constant (5 wt%) while varying the copper wt.% (xCu, where x = 8, 10, 12, 14). Several physico-chemical techniques, including X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET) analysis, scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HR-TEM), temperature-programmed desorption of ammonia (NH3-TPD), temperature-programmed reduction of hydrogen (H2-TPR), and X-ray photoelectron spectroscopy (XPS), were utilized for catalyst characterization. An environmentally friendly NiCu bimetallic-supported catalyst system was developed in response to many problems, including metal leaching, sintering, and cost. A mesoporous KIT-5 silica support with a large surface area was used. The hydrogenation of ethyl levulinate to gamma-valerolactone was studied utilizing a high-pressure stirred reactor and a range of reaction temperatures (120–160 °C), hydrogen pressures (10–30 bar), and reaction periods. Various catalysts were used in the investigation. Among all tested catalysts, the 12Cu–5Ni/KIT-5 one shows excellent activity. The best GVL yield is 84% at a conversion of 100% after 8 h of treatment at 150 °C and 25 bar H2 pressure; the promotion is also 76.1%. Optimization of reaction conditions was shown to correlate the physicochemical parameters of the catalyst with its activity.