We study the environment of the z = 6.33 ultraluminous quasar SDSS J010013.02+280225.8 (J0100) to understand its association with large-scale structure. Theoretical models propose high-redshift quasars as markers of galaxy overdensities residing in the most massive dark matter halos (DMHs) in the early Universe. J0100 is an ultraluminous quasar with the most massive black hole known at z ≳ 6, suggesting a high likelihood of residing in a massive DMH. We present wide-field (∼522 arcmin2) imaging in the r, i, and z bands from the Large Binocular Cameras on the Large Binocular Telescope, with Y- and J-band imaging from the Wide-field Infrared Camera on the Canada–France–Hawaii Telescope, centered on J0100. Applying color selections, we identify 23 objects as i-dropout Lyman break galaxy (LBG) candidates in the J0100 field. We use the deep photometric catalog in the 1.27 deg2 COSMOS field to calculate the density of LBGs in a blank field, and to estimate the selection completeness and purity. The observed surface density of LBG candidates in the J0100 field corresponds to a galaxy overdensity of δ = 4 (at 8.4σ). This large-scale overdensity suggests that the ∼22 arcmin2 overdensity found by Kashino et al. using JWST data extends out to much larger scales. We calculate the angular autocorrelation function of the candidates and find a positive correlation on ≲10′ scales as well as evidence of asymmetries in their spatial distribution, further suggesting the direct detection of large-scale structure in the field of the ultraluminous quasar J0100.