Halloysite, a naturally occurring nanoclay has unique characteristics like nanometric size range, tubular structure, high biocompatibility, low cost and opposite charges on its surface is driving attraction as a versatile and important component of biomaterials. The incorporation of functionalized Halloysite nanotubes (HNT) with the cellulose biopolymer is to obtain enhanced and desirable properties like mechanical strength, and barrier properties and to have controlled pore size. The enhanced properties of bio-nano composites are employed in wide areas including food packaging, the automobile industry, drug delivery and many more. In this chapter, extended work on various HNT-cellulose-based bio- nanocomposites is provided along with their structural, and functional properties including their applications.