This paper presents a first know study of the effect of orientation angle of carbon nanotubes (CNTs), embedded in a single-ply polymer-based CNT-reinforced composite, on buckling behavior of skew plates using an isogeometric analysis. The plate model is based on Reddy’s higher-order shear deformation theory (HSDT). Four in-plane loading conditions together with simply supported and cantilevered boundary conditions have been considered. The optimum CNT fiber orientations for CNT-reinforced composite rhombic plates with varying skew angles and boundary conditions are presented. Moreover, the effect of width-to-thickness ratio on optimum CNT orientation is explored. The results show that the efficiency of the skew plate structures can be significantly improved by simply placing the CNTs in the correct orientation.