Fabrication of traditional 3D cell culturing scaffolds requires synthetic polymers or additives, posing a risk of poor biocompatibility and low biodegradability. Pickering emulsions stabilized by biobased nanomaterials can be used as templates to produce scaffolds with facile tunable porous structure, excellent cytocompatibility, and biodegradability. In this study, very stable high internal phase Pickering emulsions (HIPPE) with an oil content of 80% were successfully prepared by xylan hydrate nanocrystals (XNC). The HIPPE can exist stably for more than 30 days, exhibiting a high viscosity. By adding cellulose nanofibers (CNF) and removing the oil phase, scaffolds with a tuned porous structure and enhanced cell culturing ability were successfully fabricated. In the HIPPE templated scaffolds with XNC/CNF, XNC plays a major role in stabilizing the emulsions, while CNF improves the mechanical properties of the scaffolds, both of which are vital to the successful fabrication of the scaffolds. Compared with non-HIPPE templated scaffolds, the HIPPE templated scaffold had a higher porosity and a higher median pore size. The HIPPE templated scaffold was able to maintain 80% cell activity and showed an excellent cytocompatibility. The HIPPE templated scaffolds consisting of XNC and CNF demonstrate great potential in 3D cell culturing for medical purpose.