ABSTRACTThe lightweight material of the thermal protection system for a reentry vehicle has become a trend in order to maximize the payload. To explore the effect of gradient density on the thermal behavior of charring materials, a pyrolysis layer model considering of variable density is developed and discretized with the central difference method. An iterative method is improved to look for the locations of the moving interfaces and boundary in each time step. Taken different gradient phenolic impregnated carbon ablator under a return trajectory heat flux for the Orion vehicle as example, their thermal behavior and effective heat capacities are simulated using the code written. Numerical results indicate that the gradient designs can improve the thermal protection performance of charring materials effectively. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 136, 47076.