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Abstract Despite the impressive performance of recent marine robots, many of their components are non‐biodegradable or even toxic and may negatively impact sensitive ecosystems. To overcome these limitations, biologically‐sourced hydrogels are a candidate material for marine robotics. Recent advances in embedded 3D printing have expanded the design freedom of hydrogel additive manufacturing. However, 3D printing small‐scale hydrogel‐based actuators remains challenging. In this study, Free form reversible embedding of suspended hydrogels (FRESH) printing is applied to fabricate small‐scale biologically‐derived, marine‐sourced hydraulic actuators by printing thin‐wall structures that are water‐tight and pressurizable. Calcium‐alginate hydrogels are used, a sustainable biomaterial sourced from brown seaweed. This process allows actuators to have complex shapes and internal cavities that are difficult to achieve with traditional fabrication techniques. Furthermore, it demonstrates that fabricated components are biodegradable, safely edible, and digestible by marine organisms. Finally, a reversible chelation‐crosslinking mechanism is implemented to dynamically modify alginate actuators' structural stiffness and morphology. This study expands the possible design space for biodegradable marine robots by improving the manufacturability of complex soft devices using biologically‐sourced materials. 

Abstract Three‐dimensional (3D) bioprinting is a promising technology to produce tissue‐like structures, but a lack of diversity in bioinks is a major limitation. Ideally each cell type would be printed in its own customizable bioink. To fulfill this need for a universally applicable bioink strategy, a versatile bioorthogonal bioink crosslinking mechanism that is cell compatible and works with a range of polymers is developed. This family of materials is termed UNIversal, Orthogonal Network (UNION) bioinks. As demonstration of UNION bioink versatility, gelatin, hyaluronic acid (HA), recombinant elastin‐like protein (ELP), and polyethylene glycol (PEG) are each used as backbone polymers to create inks with storage moduli spanning from 200 to 10 000 Pa. Because UNION bioinks are crosslinked by a common chemistry, multiple materials can be printed together to form a unified, cohesive structure. This approach is compatible with any support bath that enables diffusion of UNION crosslinkers. Both matrix‐adherent human corneal mesenchymal stromal cells and non‐matrix‐adherent human induced pluripotent stem cell‐derived neural progenitor spheroids are printed with UNION bioinks. The cells retained high viability and expressed characteristic phenotypic markers after printing. Thus, UNION bioinks are a versatile strategy to expand the toolkit of customizable materials available for 3D bioprinting.