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The interfacial properties play a crucial role in determining the performance of perovskite solar cells. We reported the effect of graphdiyne doped into both electron and hole transport layers of perovskite solar cells with an inverted structure based on MAPbI3. A peak power conversion efficiency beyond 20% was obtained with J-V hysteresis and stability remarkably improved. It reveals that the employment of doping graphdiyne not only brings out an increase of electrical conductivity, electron mobility, and charge extraction ability in the interfacial layers, but improves film morphology of the electron transport layers and reduces charge recombination which contribute to an enhanced fill factor. Later, we first employed certain amount of graphdiyne (25%) as a host material in perovskite solar cells, which is reported to successfully push the device efficiency up to 21.01%, achieving multiple collaborative effects of highly crystalline qualities, large domain sizes and few grain boundaries. Furthermore, the current-voltage hysteresis was neligible, and device stability was appreciably improved as well. It is found that graphdiyne, as the host active material, significantly affects the crystallization, film morphology and a series of optoelectronic properties of perovskite active layer, exhibiting promising applications in the field of solar cells. This study indicates that applying graphdiyne is a promising strategy to optimize the performance of perovskite solar cells.