Cellular microstructures within natural materials enlighten and promote the development of novel materials and structures in the industrial and engineering fields. Characterization of the microstructures and mechanical properties of these natural materials can help to understand the morphology-related mechanical properties and guide the structural optimization in industrial design. Among these natural cellular materials, pomelo peels, having a foam-like hierarchical microstructure, represent an ideal model for developing materials with high energy absorption efficiency. In this work, by combining X-ray tomographic imaging technique and digital volume correlation (DVC), in-situ stepwise uniaxial compression tests were performed to quantify the internal morphological evolution and kinematic responses of pomelo peel samples during compression. Via these experiments, the varying microstructure features and thus diverse resistance to compression from endocarp to exocarp are examined, and the evolution of both bundles bending and large strain domain from endocarp to mesocarp are explored. Based on the experimental results, the microstructure-related mechanical properties of pomelo peels in response to compressive loading that demonstrates nearly linear morphology-mechanics relationship were revealed.