The combustion process of Mg/PTFE/Viton-based pyrotechnics exhibits a complex multiphase flow phenomenon. However, the influence mechanism of metal particles undergoing dynamic diffusion combustion in the flow field on the infrared radiation output characteristics has not yet been elucidated. Systematic experiments and numerical simulations are performed with the combustion and infrared radiation behaviors of the pyrotechnic compositions. A small-scale sealed combustion experiment platform is specially manufactured to mimic the actual ambient pressure at different cruise altitudes. An infrared thermal imager and an infrared thermometer are adopted cooperatively to diagnose the burning process. The Euler-Langrangian method is applied to mathematically describe the gas–solid two-phase interaction in the combustion flow field, and the Eddy Dissipation Concept (EDC) combustion model is employed to simulate the coupling effect of turbulence and chemical reaction in the gas-phase reaction zone. The verified Source Six-Flux (SSF) method based in-house code solves the infrared radiative transfer equation integrating the emission, absorption and scattering effects of participating media. The comparisons with the experimental results demonstrate that the computational model involving heterogeneous reactions established in this paper better approximates the realistic situation. The results reveal that the infrared radiation output capability of dispersed combustion particles in the 2.0–5.5 μm band surpasses that of high-temperature gas molecules under different environmental pressures. The infrared radiation magnitude of both the gaseous phase and the particulate phase decrease significantly with decreasing pressure. The thermal radiation of combustion particles is mainly concentrated in the near- to mid-infrared band, while its emission in the far-infrared band is relatively weak. These scientific findings provide conducive insights for lucubrating the infrared radiation mechanism of pyrotechnics under negative pressure environments, and assist in further promoting the application of MTV pyrotechnics in the field of aerospace.