Functional gradients in hard-soft interfaces are abundant in nature, and we often mimic them to create strong and tough composites. A powerful tool for the designs and fabrication of biomimetic composites is voxel-based multi-material 3D printing. Earlier researches mainly focused on using this technique in the creation of gradients based on morphology. While this is a great way to create a gradient, the outcome material properties are often unknown. In this research, we attempted to create a gradient based on the desired outcome material properties rather than morphology. We created a linear gradient in density using a voxel-based 3D printing technique and tested it through nanoindentation. Furthermore, we created a Finite Element Model based on this sample. Out of the nanoindentation and Finite Element Model results, we extracted the b-value for a power-law function in the form of E(x)= E_h 〖ρ(x)〗^b+E_s. With the inverse of this power-law function, we designed three different gradients based on the desired material properties: a linear, stepwise, and sigmoid gradient. Nanoindentation experiments and Finite Element analyses showed that we achieved the desired outcome in material properties with our newly created approach of designing gradients. However, the nanoindentation experiments showed that using a machine suitable for the wide range of Young’s moduli present in these kinds of composites is crucial. To display the possible applications of our new approach, we designed a knee model with graded ligaments and tested it with a tensile test and digital image correlation. Results of these tests showed an energy before failure that was twice as high as its non-graded counterpart. Furthermore, with the introduction of the gradient, we achieved to change to loading condition on the ligaments. Overall, our results show that our new approach can create gradients based on material properties rather than morphology and opens many new doors in creating biomimetic composites.