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The active center of the nanomaterial is one of the main factors affecting the catalytic decomposition of ammonium perchlorate (AP), but the underlying mechanism is still not clear. In this study, we successfully replaced parts of the tetrahedral sites of MgCo2O4 with the rare earth metal element La using a one-step solution combustion synthesis method and exposed more Co3+ active centers to investigate its effect on the catalytic performance of AP. At higher Co3+/Co2+ ratios, La1%-MgCo2O4 caused a striking reduction in the THTD of AP by 215.16 °C, indicating the effect of the active center on the catalytic decomposition of AP. The successful doping of the impurity atom La also significantly enhanced the electrical conductivity of MgCo2O4 and accelerated the electron transfer process in AP thermal decomposition. More importantly, the ammonia oxidation reaction proceeds rapidly under the combined effect of La3+, O2−, high Co3+ concentration, and high electrical conductivity, leading to a quick pyrolysis of AP. In addition, the introduction of La1%-MgCo2O4 significantly shortens the ignition delay time (from 47 ms to 18 ms) of AP-based composite solid propellants (CSPs) and provides a new idea for the design of AP-based CSPs. [ABSTRACT FROM AUTHOR]