A crosslinked polyarylamide polymer exhibits novel photothermal behavior, that is, reversible giant contraction in response to near infrared irradiation in addition to normal thermal expansion. Such reversibility is seldom found in a polymeric system. Due to the amphiphilic nature of the benzocyclobutene-containing triblock copolymer precursor with polyarylamide interacting strongly with few-walled carbon nanotubes (FWCNTs), they are dispersed extremely well in the polymer solution at a loading up to at least 5 wt%. Also, strained carbon double bonds on FWCNTs can directly form covalent linkages with the benzocyclobutene groups on the polymer chains via cyclo-addition. The incorporation of FWCNTs increases mechanical stiffness two-fold. Exploiting the ability of FWCNTs to effectively convert photon energy into heat and to provide conductive pathways, the NIR-induced unexpected contraction stress can be further increased dramatically. The systematic study suggests that there is an optimal CNT concentration. At 3 wt% FWCNTs, the enhancement factor for contraction stress is almost 24: 166 kPa with 3 wt% FWCNTs versus 7 kPa without FWCNTs. The colossal photothermal contraction stress generated by this new composite film at ambient condition upon NIR stimulation can lead to the development of new NIR actuators, for example, for biological applications, and create new material platforms for green energy conversion.