We report a novel method of polyimide (PI) synthesis from prepolymers based on dianhydrides and diacetyl derivatives of aromatic diamines that facilitate the preparation of a melt processable mixture at 300 +/- 10 degrees C of the prepolymer and magnetic Nd-Fe-B alloy to provide PI-bonded magnets with enhanced properties. It is shown that chemical structure of the prepolymers strongly influences viscosity behavior via crystallization of the oligoimide in the melt, leading to formation of PI with rigid-rod like structure. This structural ordering of the prepolymers based on diacetyl derivative of diamine used in this study, if not controlled, leads to exponential increase of melt viscosity with time, making it practically impossible to prepare melt processable mixture of the magnetic particles and the PI prepolymers at elevated temperatures. The results obtained demonstrate that appropriate dianhydrides and diacetyl derivatives of diamines that do not lead to crystallization of oligoimides in prepolymer mixture can be used under controlled processing conditions to prepare melt-processable PI-bonded magnets containing rigid-rod like PI structure that significantly increases thermal stability of the magnets. The temperature dependencies of the magnetic properties of the PI-bonded magnets under conditions that they are likely to encounter during their service life were found to be remarkably similar to that of commercial thermoplastic magnets such as injection-molded nylon magnets. (c) 2006 Wiley Periodicals, Inc.