There is now the opportunity for nanomaterials to be utilized in bioapplications with low toxicity, good stability and fine dissolvability. Herein, we present a pulsed laser assisted carbon coating method for nanocrystals, and gadolinium carbide/carbon shell (GC/CS) dots with a face-centered cubic structured gadolinium carbide/core that have been synthesized in toluene. Good stability of the GC/CS dots was observed, not only in ethanol but also in the immunoconjugates. The MTT assay revealed immunoconjugates with non/low cytotoxicities. As a type of paramagnetic species, the GC/CS dots revealed excellent enhancement in magnetic resonance imaging at a high magnetic field of 14.1 T at ultra-low concentrations. In terms of the relaxivity values of the 1-3 nm GC/CS sample, both r(1) and r(2) have been dramatically increased to 86.5 mM(-1) s(-1) and 107.3 mM(-1) s(-1), respectively, thereby demonstrating the great potential for GC/CS dots to be utilized as advanced magnetic resonance agents for the diagnosis of cancers.