An oral care formulation and method for removing tartar and plaque from the teeth, gums, and oral cavity is disclosed. The oral care formulation can take the form of a toothpaste, gel, wash, rinse, soak, spray, chewing gum, dental floss, or other suitable delivery system, containing a therapeutically effective amount of dimethyl isosorbide (DMI) (or equivalent or analog thereof) and chlorine dioxide (ClO2) for removal of tartar and plaque.