binding energy, and high charge transport mobility. [1] The record power conversion efficiency of solar cells based on perovskite materials have recently reached up to 25.5%, [2] not far off traditional crystalline silicon solar cells.In a typical perovskite solar cell, the perovskite layer is sandwiched between a transparent electrode and a reflective back electrode, and electron transport layer (ETL) and hole transport layer are usually inserted between the perovskite and the electrodes to facilitate majority charge transport and to block minority charge carriers. The performance of perovskite solar cells is strongly related to the properties of the charge transport layers, especially the underneath layer on which the perovskite was cast, such as ETL in case of conventional n-i-p device architecture. In particular, the polarity of the substrates determines the nature of perovskite layer and specifically its doping state (n, p, or intrinsic) near the charge-extraction layers, [3] and the surface energy and morphology of the underneath layer affects the crystallization of the perovskite thin films. In addition, the interface issues in terms of interfacial nonradiative recombination and energy level alignment between the ETL and perovskite play an important role in the device performance, hysteresis phenomenon, and operational stability of the corresponding solar cells. [4] Furthermore, the optical constant of the underneath layer determines the light incidence and optoelectric field distribution. [5] Solution-processed tin oxide (SnO 2 ) is ubiquitously used as the electron transport layer (ETL) in perovskite solar cells, while the main concerns related to the application of SnO 2 nanoparticles are the self-aggregation potential and infeasible energy level adjustment, leading to inhomogeneous thin films and mismatched energy alignment with perovskite. Herein, a novel route is developed by adding a functional titanium diisopropoxide bis(acetylacetonate) (TiAcAc) molecule, comprising TiO 4 4core, functional CO, and long alkene groups, into the SnO 2 nanoparticle solution, to optimize the electronic transfer property of SnO 2 for efficient perovskite solar cells. It is found that the TiO 4 4can be used to tune the electronic property of the SnO 2 layer, and the long alkenes can act as a stabilizer to avoid the nanoparticle aggregation and electronic glue among the SnO 2 nanoparticles in the eventual nanoparticulate thin film, enhancing its homogeneity and conductivity. Furthermore, the residual CO groups on the ETL surface can strongly associate with the Pb 2+ and improve the interface intimacy between the ETL and perovskite. As a result, the efficiency of perovskite solar cells can be boosted from 18% to above 20% with significantly reduced hysteresis by employing SnO 2 -TiAcAc as electron transport layer, indicating a great potential for efficient perovskite solar cells.