Particle-based mesocrystals have been known for over 10 years; however, examples of biopolymer mesocrystals are rather scarce. The synthesis of particle precursors of biopolymers, the identification of particle-mediated crystallization processes, and thus the synthesis of mesocrystals of biopolymers are challenging. Here, we summarize the existing examples of biopolymer crystallization based on self-assembly of the secondary structures, which could induce the formation of biopolymer mesocrystals. As basic building units, simple secondary structures such as β-sheets or α-helixes could provide a useful tool for the design of biopolymer mesocrystals.