transport dynamics, which is the key for high-performance perovskite devices. At present, precursor solution additive as a convenient and effective method has been widely used in the structural optimization of perovskite films, [8] such as doping in the perovskite lattice to form bonds, [9] and additives to form hydrogen bonds with perovskites. [10] Quantum dots (QDs) are often doped in perovskite grain boundaries to reduce the boundary barrier for promoting the transport of photogenic carriers. [11] In addition, additives to prevent water/oxygen penetration by forming strong chemical bonds at the interface are important way to improve the stability of perovskite films. [12] Although precursor solution additive method provides an excellent material based for the structural optimization, the current postprocessing methods are limited to fabricate crystalline perovskite films to control their structure and properties, due to the challenges in manipulate the heating/cooling rate, residual stress, and microstructure, such as grain size, intragrain defects, and grain boundary defects. Laser has been widely used in semiconductor processing because of its advantages of monochromatism, coherence, directionality, high speed processing, scalability, wide range control of energy density, and wavelength. The laser-assisted processing technology was developed for rapid processing of perovskite, [13] which can facilitate the postprocessing of perovskite devices with high speed. Moreover, compared with the traditional thermal annealing, the energy consumption of laser treatment is much less. [14] In addition, The temperature control at the material interface, such as grain boundaries, is critical for defect density, and phases, which are important for high-performance perovskite-based optoelectronic devices. However, it is challenging to fine-tune the microstructures in perovskite films with well-controlled grain structure, interface defects, porosity, phase structure, and strains, simultaneously. Here, pulsed laser technology is combined with carbon quantum dots (CQDs) into perovskite absorbers with pore-free, less defect, high crystallinity, enhanced absorption, low stress, and phase-stabilized microstructures. Due to laser-CQD interaction-induced grain boundary microstructure changes, perovskite films can be fabricated with much larger grains (>10 times) than those after thermal annealing. As CQDs are embedded to passivate grain, this leads to reduced grain boundary barrier at the interface, which significantly improve the carrier transportation in perovskite films. The shift of perovskite band to vacuum energy level leads to remarkable improvement of carrier extraction efficiency and lifetime, leading to much higher mobility of photogenerated carriers and diffusion length (>1 μm). The laser-induced thermomechanical momentum significantly enhances crystal interface with hydrophobic perovskite film, resulting in much less residual tensile stress by 20 times and excellent stability. Pulsed-laser-assisted QD additive engineerin...