We report the solid-state reaction of MoO 2 nanosheets, obtained from the soft-chemical delamination of Na 0.9 Mo 2 O 4 , into metallic Mo 2 C single layers that constitute a new family of versatile carbide nanosheets. This so-called pseudotopotactic reaction, i.e., conversion from nanosheet to nanosheet, is aided by the use of cationic polymers as binders for the film growth based on electrostatic self-assembly. Compared to Mo 2 C in the bulk form, 2D anisotropic Mo 2 C sheets having a larger surface-area-to-volume ratio are of significant use in potential electrochemical applications, and it is also worth noting that the thickness of Mo 2 C sheets can be controlled in the nanometer range by altering the stacking number of the precursor nanosheets.