The electric-quadrupole coupling constant of the ground states of the proton drip line nucleus $^{20}$Na($I^{pi}$ = 2$^{+}$, $T_{1/2}$ = 447.9 ms) and the neutron-deficient nucleus $^{21}$Na($I^{pi}$ = 3/2$^{+}$, $T_{1/2}$ = 22.49 s) in a hexagonal ZnO single crystal were precisely measured to be $|eqQ/h| = 690 pm 12$ kHz and 939 $pm$ 14 kHz, respectively, using the multi-frequency $beta$-ray detecting nuclear magnetic resonance technique under presence of an electric-quadrupole interaction. A electric-quadrupole coupling constant of $^{27}$Na in the ZnO crystal was also measured to be $|eqQ/h| = 48.4 pm 3.8$ kHz. The electric-quadrupole moments were extracted as $|Q(^{20}$Na)$|$ = 10.3 $pm$ 0.8 $e$ fm$^2$ and $|Q(^{21}$Na)$|$ = 14.0 $pm$ 1.1 $e$ fm$^2$, using the electric-coupling constant of $^{27}$Na and the known quadrupole moment of this nucleus as references. The present results are well explained by shell-model calculations in the full $sd$-shell model space.
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