To fully understand the role of xyloglucan (XyG) on the microstructural and mechanical properties of pectin cryogels, we formulated two types of low methoxyl pectin cryogels containing different XyG content (with or without an ionic network) using freeze-drying. The interaction between the pectin and XyG was explored, and the morphologies of ice crystals were characterized by the pore morphometric of freeze-dried scaffolds. Results showed that XyG and pectin could be cross-linked via hydrogen bonding interactions. When the ionic network was present, XyG accelerated pectin gelation but decreased the size of ice crystals during freezing, reducing the pore diameters of cryogels from 340 to 350 µm to 210-230 µm while shifting the structural thickness from 50 to 70 µm to 30-50 µm. When the ionic network was absent, the addition of XyG increased the pore size of the pectin cryogel from 30 to 50 µm to 70-90 µm, while rising the pore wall thickness from 50 to 70 µm to 70-90 µm. The ionic cross-links between the pectin chains gave freeze-dried scaffolds mechanical strength and crispiness, and the incorporation of XyG further strengthened the mechanical resistance of cryogels.