Purpose <p>To evaluate the relationships between the magnitudes of corneal asymmetry and induced ocular higher-order aberrations (HOAs) after small-incision lenticule extraction (SMILE) for moderate-to-high myopia.</p> Methods <p>Sixty-six eyes of 66 patients who underwent SMILE were divided into two groups: the high (SE ≥ -6.0 D, n = 27, Group H) and moderate (−&#xa0;3.0 D ≤ SE &lt; −&#xa0;6.0 D, n = 39, Group M) myopia groups. Using Fourier harmonic analysis, the spherical component (SC), regular astigmatism (RA), asymmetry, and higher-order irregularity (HOI) were obtained from videokeratography data. Visual acuity, manifest refraction, and ocular HOAs were assessed at baseline and 3, 6, and 12&#xa0;months postoperatively. The relationships between Fourier components and ocular HOAs were assessed.</p> Results <p>In both groups, vertical coma, horizontal coma, spherical aberration, total higher-order aberrations (tHOAs), and asymmetry of the anterior corneal surface increased postoperatively (from 3 to 12&#xa0;months), while SC and RA of the anterior corneal surface decreased (all <i>P</i> &lt; 0.05). More vertical coma and asymmetry of the anterior corneal surface were induced in Group H than in Group M at 3 and 6&#xa0;months postoperatively (all <i>P</i> &lt; 0.05). The association between preoperative asymmetry of the anterior corneal surface and preoperative spherical aberration was significant in both groups (R² = 0.138, <i>P</i> = 0.02; R² = 0.172, <i>P</i> = 0.032, respectively). The asymmetry of the anterior corneal surface was correlated with vertical coma, spherical aberration, and tHOAs at 3, 6, and 12&#xa0;months postoperatively in both groups (all R² &gt; 0.2, all <i>P</i> &lt; 0.05).</p> Conclusions <p>The visual quality after SMILE was associated with the asymmetry of the anterior corneal surface for moderate and high myopia.</p>