A facile, cost-effective and scaleable method is presented for the fabrication of thin film α-MoO3/SWCNT-COOH composite electrodes with a high charge storage capacity in LiClO4/propylene carbonate in a 1.5–3.5V (versus Li/Li+) working electrochemical window. α-MoO3 nanobelts were synthesized using an established hydrothermal method and composite thin film electrodes incorporating interwoven single walled carbon nanotubes as an electrical conductive additive within a network of α-MoO3 nanobelts were manufactured by spray deposition. The composite electrode showed a maximum charge storage/capacitance of 697.7Cg−1 (193.8mAhg−1)/ 348.7Fg−1 at 0.1mVs−1 (per unit mass of composite electrode) with a contribution to charge storage from capacitive and diffusion controlled processes of 443Cg−1 and 463.2Cg−1 (per unit mass of α-MoO3), respectively, which is comparable to charge storage attained by electrodes manufactured by more costly and non-scaleable templating methods previously reported. Cyclic voltammetry showed capacitances of 167Fg−1 and 75Fg−1 at 10mVs−1 and 50mVs−1, respectively, suggesting a potential application as electrochemical capacitor electrodes of moderate power densities. On the other hand, a charge storage of 697.7Cg−1 (193.8mAhg−1) attained at 0.1mVs−1, and a capacity of 596.8mAhg−1 achieved at 10mAg−1 in galvanostatic charge–discharge experiments supports a potential application of α-MoO3 as a Li-ion battery cathode.