Laser ignition of energetic material composites was studied for initiation with heating rates from 9.5 × 104 to 1.7 × 107 K/s. This is a unique heating rate regime for laser ignition studies because most studies employ either continuous wave CO2 lasers to provide thermal ignition or pulsed Nd:YAG lasers to provide shock ignition. In this study, aluminum (Al) and molybdenum trioxide (MoO3) nanoparticle powders were pressed into consolidated pellets and ignited using a Nd:YAG laser (1064 nm wavelength) with varied pulse energy. Results show reduced ignition delay times corresponding to laser powers at the ablation threshold for the sample. Heating rate and absorption coefficient were determined from an axisymmetric heat transfer model. The model estimates absorption coefficients from 0.1 to 0.15 for consolidated pellets of Al + MoO3 at 1064 nm wavelength. Ablation resulted from fracturing caused by a rapid increase in thermal stress and slowed ignition of the pellet.