We have fabricated carbon nanotube (CNT)-polyurethane (TPU) sheets via a one-step filtration method that uses a TPU solvent/non-solvent combination. This solution method allows for control of the composition and processing conditions, significantly reducing both the filtration time and the need for large volumes of solvent to debundle the CNTs. Through an appropriate selection of the solvents and tuning the solvent/non-solvent ratio, it is possible to enhance the interaction between the CNTs and the polymer chains in solution and improve the CNT exfoliation in the nanocomposites. The composition of the nanocomposites, which defines the characteristics of the material and its mechanical properties, can be precisely controlled. The highest improvements in tensile properties were achieved at a CNT:TPU weight ratio around 35:65 with a Young’s modulus of 1270 MPa, stress at 50 % strain of 35 MPa, and strength of 41 MPa, corresponding to ~10 fold improvement in modulus and ~7 fold improvement in stress at 50 % strain, while maintaining a high failure strain. At the same composition, CNTs with higher aspect ratio produce nanocomposites with greater improvements (e.g. strength of 99 MPa). Electrical conductivity also shows a maximum near the same composition, where it can exceed the values achieved for the pristine nanotube buckypaper. The trend in mechanical and electrical properties was understood in terms of the CNT-TPU interfacial interactions and morphological changes occurring in the nanocomposite sheets as a function of increasing the TPU content. The availability of such a simple method and the understanding of the structure-properties relationship are expected to be broadly applicable in the nanocomposites field.