The noncontact crucible method was used to prepare square Si single bulk crystals. The size of the square part of the ingots was determined by the side-face width of the four-cornered pattern that appeared on the top surface. We obtained square Si single crystals with sizes of 9.4 × 9.7 and 10.9 × 11.0 cm2 that had no fan-shaped {110} faces and had diagonal lengths of up to 91% of the crucible diameter. To obtain large square Si single bulk crystals with a large side-face width using the present method, the importance of establishing a larger low-temperature region in the Si melt while maintaining a smaller initial temperature reduction was considered.