Chitosan possesses beneficial properties such as its biodegradability, biocompatibility, and adsorption of metallic ions, which make it attractive in various applications. In addition, besides excellent mechanical and electrical properties, carbon nanotubes have been reported to be biocompatible platforms for neuronal growth and differentiation. In this work, porous carbon nanotubes/chitosan (CNTs/CHI) composites are prepared by unidirectional freezing CNTs dispersion in chitosan aqueous solution and subsequent freeze drying, which is named as ice-templating. Two types of macroscopic shapes with high and low aspect ratio are produced by immersion freezing and one-side contact freezing respectively. The SEM characterization indicates that the produced CNTs/CHI composites are composed of a three dimensional network with lamellar structure and macropores in micron scale, and the products by two freezing styles have different micro-structural characters. The produced CNTs/CHI composite has a very low density and self-standing ability, which makes it having very good permeability and processability. It is anticipated that the CNTs/CHI composites have various applications such as conductive network in polymer, biological carrier, catalyst supports, adsorbents, and permeable membranes.