We prepared gadolinium oxide (Gd2O3) nanoparticles (GNPs) coated with a trans‐activator of transcription (TAT) peptide with cell‐penetrating ability (i.e., TAT‐GNPs) through one‐pot process. We characterized the particle diameter, surface‐coating structure, water proton relaxivities, and in vitro cellular toxicities of the TAT‐GNPs. We measured in vivo T1 magnetic resonance images (MRI) in a model nude mouse with liver cancer prior and posterior to intravenous administration. The average particle diameter of the GNPs was 1.5 nm. The sample solution exhibited a longitudinal water proton relaxivity (r1) of 18.2/s/mM (r2/r1 = 1.6, r2 = transverse water proton relaxivity), which is four to five times higher than those of commercial Gd‐chelates. The in vivo T1 MRI exhibited positively (or T1) enhanced contrasts in the mouse liver cancer after intravenous administration, demonstrating that the TAT‐GNPs acted as an enhanced cancer‐imaging agent similar to the cancer‐targeting agent in T1 MRI.