Self-assembling proteins are valuable building blocks allowing the construction of materials with versatile chemical properties and functions based on their tertiary and quaternary protein structures. Well-studied motifs from tandem repeat proteins (such as silk, elastin, collagen, keratin, resilin, and squid ring teeth-SRT) have been frequently used in combination to create multifunctional materials for diverse applications. Besides their extraction from natural sources, these biopolymers are produced using genetically modified organisms. Such materials and their engineered derivatives via directed evolution can exhibit extraordinary physical responses that have not been observed in synthetic or inorganic materials. Those properties and responses selected via directed evolution can play significant roles in achieving novel functionalities and fabricating various devices. In the last decade, we discovered that tandem repeat biopolymers can be tuned for predefined macroscopic symmetries, which cannot be obtained in traditional materials engineering, by controlling their packing symmetry or order during assembly. In this talk, we review programmable design, structure, and properties of functional fibers and films from squid-inspired tandem repeat proteins, for the design of thermal, structural and optical biological materials [1-3].