The consumption of plant-based proteins sourced from pulses is sustainable from the perspective of agriculture, environment, food security, and nutrition. Increased incorporation of high-quality pulse ingredients into foods such as pasta and baked goods is poised to produce refined food products to satisfy consumer demand. However, a better understanding of pulse milling processes is required to optimize the blending of pulse flours with wheat flour and other traditional ingredients. A thorough review of the state-of-the-art on pulse flour quality characterization reveals that research is required to elucidate the relationships between the micro-and nanoscale structures of these flours and their millingdependent properties, such as hydration, starch and protein quality, components separation, and particle size distribution. With advances in synchrotron-enabled material characterization techniques, there exist a few options that have the potential to fill knowledge gaps. To this end, we conducted a comprehensive review of four high-resolution nondestructive techniques (i.e., scanning electron microscopy, synchrotron X-ray microtomography, synchrotron small-angle X-ray scattering, and Fourier-transformed infrared spectromicroscopy) and a comparison of their suitability for characterizing pulse flours. Our detailed synthesis of the literature concludes that a multimodal approach to fully characterize pulse flours will be vital to predicting their end-use suitability. A holistic characterization will help optimize and standardize the milling methods, pretreatments, and post-processing of pulse flours. Millers/processors will benefit by having a range of well-understood pulse flour fractions to incorporate into food formulations.