Concentration- and layer-dependent percolation thresholds can be determined for carbon nanotube (CNT) films deposited from aqueous dispersions on paper substrates at both the surface of the deposited film (in-plane) and through the thickness of the paper (thru-plane) using impedance spectroscopy. By analyzing the impedance spectra as a function of the number of layers (solution concentration is constant) or the solution concentration (number of layers is constant), the electrical properties and percolation thresholds for CNT-paper composites can be determined. In-plane measurements show that percolation occurs at 4 layers when 1 mg/mL solution concentration is used. In the thru-plane direction, the films are already percolated at 1 mg/mL concentration, which is confirmed by varying the concentration of the solution used to deposit 1 layer films. A second percolation event happens between 8 and 12 layers due to an increased number of interconnections of CNTs within the paper substrate. The lowest sheet resistance achieved was 100 Ω/□.