Anisotropic plasmonic films are a desirable material for many optoelectronic ap-plications. Here, we propose a method to align silver nanowires (AgNWs) with the help of uniaxial nematic alignment of cellulose nanocrystal (CNC) liquid crystals (LCs) that can preserve their LC orientation in solid film. AgNWs are doped into uniaxial nematic CNC LCs, where AgNWs are oriented parallel to the director of shear-aligned CNCs without aggregation. The AgNWs orientations are determined by polarized optical and dark field microscopic images. The alignment of AgNWs is characterized by the scalar order parameter S , and the measured S around 0.59 for aligned AgNWs presents an improved anisotropy with the assistance of uniaxial nematic CNC LCs. The electrical property of aligned AgNWs is examined by the four-probe method and exhibits the maximum ratio of anisotropic sheet resistance around 5, consistent with the simulated percolation probability performance using the Monte Carlo computation. Our results show that the uniaxial nematic CNC LCs can act as an effective template in aligning AgNWs, which is compatible with 3D printing and microfluidics, and allows for the preparation of low-cost, innovative optical materials and devices.