A treatment agent for chromium-free insulating coating formation suitable for forming an insulating coating on a surface of a grain-oriented electrical steel sheet. The treatment agent includes components (A), (B), (C), and (D). The component (B) is contained in an amount of 50 to 150 parts by mass on a SiO2 solid basis, and the component (C) is contained in an amount of 5.0 parts by mass or more on an elemental metal basis, the amounts being based on 100 parts by mass, on a solid basis, of the component (A). The component (D) is contained in an amount that a molar ratio of M2+ and M3+, each being a metal element in the treatment agent for chromium-free insulating coating formation, to a phosphorus element P satisfies a specified relationship, and the treatment agent for chromium-free insulating coating formation has a pH of less than 4.5.