Conversion of biomass‐derived furfural platform compound to value‐added tetrahydrofurfuryl alcohol (THFL) molecule is a sustainable route, and an efficient nonnoble metallic catalyst is a key factor for this reaction. In this work, Ni@C@CNT composite as a highly effective catalyst for hydrogenation of furfural to tetrahydrofurfuryl alcohol was synthesized by one‐step pyrolysis of Ni‐centered metal organic framework (Ni‐MOF) doping with carbon nanotube (CNT). For comparison, Ni@C catalyst derived directly from Ni‐MOF was also synthesized. The characterization results show that the doping of CNT promotes high dispersion of active sites and formation of Ni3C phase which has Pt‐like catalytic activity. Therefore, the obtained Ni@C@CNT exhibited excellent activity in furfural hydrogenation (99.1% furfural conversion and 94.7% THFL yield at 120°C, 4 h, 4‐MPa initial hydrogen pressure). Ni@C@CNT also shows good stability in reuse test. Current work presents a facile method for preparation of nonnoble metallic catalysts with high efficiency.