Hydrolyzed nitrilotriacetonitrile compositions are disclosed prepared by a method characterized by a one-shot addition of an amount of nitrilotriacetonitrile to a solution containing an acid catalyst, where the reaction is complete in a time period of less than an hour. The method is also characterized by adjusting the pH of the reaction mixture to a pH of at least 8. The method is also characterized by oxidatively removing free cyanide to a desired low level through the addition of an oxidizing agent the produces environmentally benign by-products to the crude hydrolyzed NTAN to form hydrolyzed NTAN compositions having minimized, negligible, or substantially no free cyanide levels.