The gradient of surface temperature is known as Marangoni convection and plays an important role in silicon melt, spray, atomic reactors, and thin fluid films. Marangoni convection has been considered in the liquid film spray of carbon nanotube (CNT) nanofluid over the unsteady extending surface of a cylinder. The two kinds of CNTs, single-wall carbon nanotubes (SWCNTs) and multiple-wall carbon nanotubes (MWCNTs), formulated as water-based nanofluids have been used for thermal spray analysis. The thickness of the nanofluid film was kept variable for a stable spray rate and pressure distribution. The transformed equations of the flow problem have been solved using the optimal homotopy analysis method (OHAM). The obtained results have been validated through the sum of the total residual errors numerically and graphically for both types of nanofluids. The impact of the physical parameters versus velocity, pressure, and temperature pitches under the influence of the Marangoni convection have been obtained and discussed. The obtained results are validated using the comparison of OHAM and the (ND-solve) method.