Natural rubber (NR) composites containing bio-based chitin nanofibers (ChNFs) exhibit a wide range of mechanical properties - from rubber to plastic behavior - with increasing chitin contents. A constrained 3-dimensional network can be formed by mixing natural rubber latex and a modified zwitterionic rigid chitin counterpart. By inclusion of highly anisotropic chitin nanofibers (30 wt%), strain-induced NR crystallization occurs at a much lower strain of 50%. More intriguingly, 2D-WAXD results reveal that the strain-induced crystallization of NR/ChNFs composites show 3-dimensionally oriented crystallite formation behaving similar to "3D-single crystals orientation" when the content of ChNFs is over 5 wt%. It is suggested that not only c-axis (NR chains) orients along the stretching direction, but also the a- and b-axes deliberately arrange along the normal direction and transverse direction, respectively. Structure and morphology in 3-dimensional spaces after strain-induced crystallization of the NR/ChNFs30 composite are investigated in detail. Therefore, this study might pave a new way to enhance mechanical properties by incorporation of ChNFs, obtaining 3-dimensionally oriented crystallites of novel multifunctional NR/ChNFs composite with shape memory ability.