The authors report a method where in-situ photon assisted heating of multi-wall carbon nanotubes was utilized for enhanced polymerization of the nanotube/polydimethylsiloxane interface that resulted in significant load transfer and improved mechanical properties. Large Raman shifts (20 cm(-1) wavenumbers) of the 2D bands were witnessed for near-infrared light polymerized samples, signifying increased load transfer to the nanotubes for up to ∼80% strains. An increase in elastic modulus of ∼130% for 1 wt. % composites is reported for photon assisted crosslinking.