The oil-soluble iron-nickel bimetallic catalyst precursor was synthesized for the application of coal/oil co-processing. The catalyst precursor and its sulfurized product were characterized by FTIR, TG, XRD, and TEM. And the catalytic performance of this catalyst precursor in the coal/oil co-processing system was investigated and compared with the molybdenum naphthenate. The results showed that the average particle size of the synthesized catalyst precursor after sulfurization was about 40 nm, containing (Fe, Ni)(9)S-8 mixed crystal, and the crystallinity was low with rough edge and large specific surface area. The synthesized catalyst precursor showed better hydrogenation activity compared with the relatively expensive molybdenum naphthenate catalyst. Under the experimental conditions, the yield of coke was only 2.9 wt%, the I value was 6.47, and the conversion yield of dry ash-free coal reached to 90.7 wt%. Characterization and analysis of the coke after reaction further confirmed that the synthesized catalyst precursor could promote the conversion of coal and showed potential application value in coal/oil co-processing.