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Multilayered multi‐material interfaces are encountered in an array of fields. Here, enhanced mechanical performance of such multi‐material interfaces is demonstrated, focusing on strength and stiffness, by employing bondlayers with spatially‐tuned elastic properties realized via 3D printing. Compliance of the bondlayer is varied along the bondlength with increased compliance at the ends to relieve stress concentrations. Experimental testing to failure of a tri‐layered assembly in a single‐lap joint configuration, including optical strain mapping, reveals that the stress and strain redistribution of the compliance‐tailored bondlayer increases strength by 100% and toughness by 60%, compared to a constant modulus bondlayer, while maintaining the stiffness of the joint with the homogeneous stiff bondlayer. Analyses show that the stress concentrations for both peel and shear stress in the bondlayer have a global minimum when the compliant bond at the lap end comprises ≈10% of the bondlength, and further that increased multilayer performance also holds for long (relative to critical shear transfer length) bondlengths. Damage and failure resistance of multi‐material interfaces can be improved substantially via the compliance‐tailoring demonstrated here, with immediate relevance in additive manufacturing joining applications, and shows promise for generalized joining applications including adhesive bonding. [ABSTRACT FROM AUTHOR]