Perovskite crystal grain size control, grain boundary passivation, and grain bridging are the keys to obtaining high efficiency in perovskite solar cells. A small amount of semi-conducting single-walled carbon nanotubes added to a perovskite active layer can achieve this. In particular, the surfactants attached to the semiconducting single-walled carbon nanotubes a crucial role. In this work, we synthesized a new surfactant, 4,6-di(anthracen-9-yl)-1,3-phenylene bis(dimethylcarbamate), which has a polyaromatic group on one end and a urea-analogue carbamate group on the other end. The polyaromatic anthracene end functions as a nanotweezer clenching the carbon nanotubes strongly via pi-pi interaction while the carbamate end interacts with Pb2+, functioning as a strong Lewis base. In addition, the new surfactant has conjugated double bonds with a suitable bandgap, resulting in enhanced charge mobility in the perovskite film. Overall, the new surfactant-clenched semiconducting carbon nanotubes showcase superior effectiveness as passivators and charge bridges in perovskite solar cells as compared to the conventional deoxycholate surfactant-wrapped semiconducting single-walled carbon nanotubes. The new surfactant-attached semiconducting carbon nanotube-added NH3CH3PbI3-based perovskite solar cells exhibited a power conversion efficiency of 20.7%, which is higher than that of the reference devices with no additives (18.4%) and the previously reported semiconducting single-walled carbon nanotube-added devices (19.7% in this work and 19.5% in the literature).