Comb-like polymers with flexible side chains chemically pended onto a polymeric backbone afford some unusual properties due to their hierarchical structures, such as nanoscale confined crystallisation, phase transition and conformational variations, length scale effects, etc. Considerable attention has been paid to these featured polymers, regarding their importance in understanding the correlation between hierarchical structure and the assembled morphologies. In this review, we reviewed the recent research progress on the structure–property correlations of comb-like polymers. This article brings together and highlights the fabrication, structure determination and morphology characterization for comb-like polymers, especially for nanostructured packing patterns and frustrated mobility of chain segments from the selected examples.