As a two-dimensional material, graphene has attracted increasing attention as heat dissipation material owing to its excellent thermal transport property. In this work, we fabricated sisal nanocrystalline cellulose/functionalized graphene papers (NPGs) with high thermal conductivity by vacuum-assisted self-assembly method. The papers exhibit in-plane thermal conductivity as high as 21.05 W m-1 K-1 with a thermal conductivity enhancement of 403% from the pure cellulose paper. The good thermal transport properties of NPGs are attributed to the strong hydrogen-bonding interaction between nanocrystalline cellulose and functionalized graphene and the well alignment structure of NPGs.