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Abstract Shear‐recoverable hydrogels based on block copolypeptides with rapid self‐recovery hold potential in extrudable and injectable 3D‐printing applications. In this work, a series of 3‐arm star‐shaped block copolypeptides composed of an inner hydrophilic poly(l‐glutamate) domain and an outer β‐sheet forming domain is synthesized with varying side chains and block lengths. By changing the β‐sheet forming domains, hydrogels with diverse microstructures and mechanical properties are prepared and structure–function relationships are determined using scattering and rheological techniques. Differences in the properties of these materials are amplified during direct‐ink writing with a strong correlation observed between printability and material chemistry. Significantly, it is observed that non‐canonical β‐sheet blocks based on phenyl glycine form more stable networks with superior mechanical properties and writability compared to widely used natural amino acid counterparts. The versatile design available through block copolypeptide materials provides a robust platform to access tunable material properties based solely on molecular design. These systems can be exploited in extrusion‐based applications such as 3D‐printing without the need for additives.