Co–Fe–Al catalysts prepared using coprecipitation at laboratory scale were investigated and extended to pilot scale for high-calorific synthetic natural gas. The Co–Fe–Al catalysts with different metal loadings were analyzed using BET, XRD, H2-TPR, and FT-IR. An increase in the metal loading of the Co–Fe–Al catalysts showed low spinel phase ratio, leading to an improvement in reducibility. Among the catalysts, 40CFAl catalyst prepared at laboratory scale afforded the highest C2–C4 hydrocarbon time yield, and this catalyst was successfully reproduced at the pilot scale. The pelletized catalyst prepared at pilot scale showed high CO conversion (87.6%), high light hydrocarbon selectivity (CH4 59.3% and C2–C4 18.8%), and low byproduct amounts (C5+: 4.1% and CO2: 17.8%) under optimum conditions (space velocity: 4000 mL/g/h, 350 °C, and 20 bar).