CNTs are exceptional support materials for heterogeneous catalysis. Their large specific surface areas readily disperse nanoparticles to avoid agglomeration, and their high electronic conductivities make them promising for electrochemical applications. Herein, we present new insights into the role of CNTs in heterogeneous catalysis. Thanks to recent advancements in synthesis and purification, the diameters of CNTs can be controlled from 2 nm to >50 nm, making them ideal supports for inducing strain in sub-2 nm planar molecules. Depending on the local interactions between curved CNTs and the overlayer, molecules may undergo controllable distortion to alleviate strain (Fig. ). Assuming the overlayer is fully elastic and the interlayer distance is 0.3 nm, the bending angle can range from ~96 o (1 nm-diameter CNT) to ~1.5 o (100 nmdiameter CNT) (See Supplementary Methods 1 for estimates). We report X-ray spectroscopic studies and other spectra to assess the structure of molecular CoPc before and after monodispersion on various CNTs. We observe significant molecular distortion and strong molecule-CNT interactions for SWCNTs. This is supported by our DFT calculations that find increased distortion strengthens Co-CO binding, which improves selectivity towards MeOH. As a result, the distorted CoPc/SWCNT exhibits a 385% improvement in FEMeOH compared to CoPc/MWCNT. We also extend these findings to ORR and CO2RR studies on SWCNTs, which also exhibit straindependent catalytic activity.