Ice-templating method is also known as directional freezing or freeze-casting. Its principle is to use the ice crystals formed in the freezing process as a template, sublimate the solvent through post decompression, and then densify it through post-treatment, and finally obtain the bionic structure. This method has the advantages of strong controllability of microstructure, wide application range of raw materials, and the ability to prepare large-scale materials, which is widely used in the preparation of directional control ceramics, polymers, metals, and carbon materials. Exploring the impact mechanisms of controlling functional nanomaterials to assemble composite materials by ice-templating method, and analyzing the interaction relationship of ice-templating method with other materials’ processing methodologies, is of great significance for improving material properties and developing new materials. This review describes fundamental principles, synthesis strategies, and pore regulation of the preparation of multi-scale complex bionic structural materials by ice-templating method. Focusing on the nucleation and growth of ice crystals, it summarizes the measures to control the pore structure of ice-templating method. In addition, it outlines the assisted construction of pore geometries by ice-templating method. Finally, the correlation between the microstructure and macromorphology of the composites is analyzed in-depth, highlighting the influence mechanism of different freezing processes on the pore structure, and prospects for future directions in this field.