Additive manufacturing of cellulose-based materials with continuous, multidirectional stiffness gradients

Functionally graded materials (FGMs) enable applications in fields such as biomedicine and architecture, but their fabrication suffers from shortcomings in gradient continuity, interfacial bonding, and directional freedom. In addition, most commercial design software fail to incorporate property gradient data, hindering explorations of the design space of FGMs. Here, we leveraged a combined approach of materials engineering and digital processing to enable extrusion-based multimaterial additive manufacturing of cellulose-based tunable viscoelastic materials with continuous, high-contrast, and multidirectional stiffness gradients. A method to engineer sets of cellulose-based materials with similar compositions, yet distinct mechanical and rheological properties, was established. In parallel, a digital workflow was developed to embed gradient information into design models with integrated fabrication path planning. The payoff of integrating these physical and digital tools is the ability to achieve the same stiffness gradient in multiple ways, opening design possibilities previously limited by the rigid coupling of material and geometry.