The successful fabrication of freestanding two-dimensional (2D) crystals that exhibit unprecedented high crystal quality and macroscopic continuity renovates the conventional cognition that 2D long-range crystalline order cannot stably exist at finite temperatures. Current progresses are primarily limited to van der Waals (vdW) layered materials, while studies on how to obtain 2D materials from nonlayered bulk crystals remain sparse. Herein, we report the experimental realization of vdW-like cubic ZrN single crystal and emphasize the significant role of confined electrons in stabilizing the atomic structure at the 2D limit. Furthermore, the exfoliated ZrN single-crystal films with a few nanometers thick exhibit dimensional crossover effect of emerging 2D superconductivity with the unconventional upper critical field beyond Pauli paramagnetic limit, which suggests a dimensional effect in the pairing mechanism of dimensionally confined superconductors.