The thermal and mechanical, near-resonant responses of particulate composite plates formed from hydroxyl-terminated polybutadiene (HTPB) binder and varying volume ratios of ammonium chloride (NH4Cl) particles (50, 65, 75%) are investigated. Each test specimen is clamped and forced with three levels of band-limited, white noise inertial excitation (10–1000 Hz at 1.00, 1.86 and 2.44 g RMS). The mechanical response of each plate is recorded via scanning laser Doppler vibrometry. The plates are then excited at a single resonant frequency and the thermal response is recorded via infrared thermography. Comparisons are made between the mechanical operational deflection shapes of each plate and spatial temperature distributions, with correlation seen between the observed level of strain, as visualized by strain energy density, and heat generation. The effect of particle/binder ratio on both the thermal and mechanical responses is discussed. Acquired results are also compared to an analytical model of the system. The observed thermomechanical effects render an improved understanding of the thermomechanics of plastic-bonded composites, an essential step in support of the development of new technologies for the vapor-based detection of hidden explosives.