The development of noninvasive imaging techniques for the accurate diagnosis of progressive hepatocellular carcinoma (HCC) is of great clinical significance and has always been desired. Herein, a hepatocellular carcinoma cell-targeting fluorescent magnetic nanoparticle (NP) was obtained by conjugating near-infrared fluorescence to the surface of FeO (NIRF-FeO) NPs, followed by coating the lipids consisting of tumoral hepatocytes-targeting polymer (Gal-P). This magnetic NP (GPC@NIRF-FeO) with superparamagnetic behavior showed high stability and safety in physiological conditions. In addition, GPC@NIRF-FeO achieved more specific uptake of human liver cancer cells than free FeO NPs. Importantly, with superpara-magnetic iron oxide and strong NIR absorbance, GPC@NIRF-FeO NPs demonstrate prominent tumor-contrasted imaging performance both on fluorescent and T-weighted magnetic resonance (MR) imaging modalities in a living body. The relative MR signal enhancement of GPC@NIRF-FeO NPs achieved 5.4-fold improvement compared with NIR-FeO NPs. Therefore, GPC@ NIRF-FeO NPs may be potentially used as a candidate for dual-modal imaging of tumors with information covalidated and directly compared by combining fluorescence and MR imaging.