received much attention recently due to its excellent photoelectric properties, such as strong light-absorbing coefficient, long carrier lifetime, adjustable bandgap and simple fabrication process. [3-9] In the past few years, the power conversion efficiency (PCE) of perovskite solar cells (PSCs) has been promoted from 3.8% to 25.2% by the substantial effort, such as the additive engineering, interface engineering, and film morphology engineering. [10-14] However, the mesoporous PSCs require high sintering temperature, increasing energy consumption and device cost, which are incompatible with commercial and flexible applications. [15-17] Hence numerous efforts are conducted to fabricate the planar PSCs with well-established low-temperature and simple fabrication process. [18-20] Unfortunately, researches have shown that perovskite films in the planer PSCs prepared by one-step anti-solvent deposition have many interface defects, [21-24] which accelerate the degradation of PSCs under humidity, oxygen, thermal condition and illumination fields. [25-28] Thus, interface modification is extensively used to improve the photovoltaic performance of the PSCs. [29-33] In planar PSCs, the electron transfer layer (ETL) and hole transport layer (HTL) have crucial influences on the crystallization process of perovskite films. Meanwhile, the interfacial contacts between the ETL (or HTL) and the perovskite films affect the photogenerated carriers dynamic and thus change the overall device efficiency, stability and hysteresis. [34-38] It is well known that the enlarged grains of perovskite films and decreased interface defects boost the performance of PSCs. Accordingly, the interface modification at perovskite/HTL and perovskite/ETL interfaces have been investigated and optimized. For instance, several effective electronic transport materials (i.e., TiO 2 , ZnO, SnO 2) have been modified by inserting a passivation layer to aggrandize grain size, reduce interface recombination and increase interface carrier transmission in normal planar PSCs. [39-43] For the inverted PSCs, several organic and inorganic materials formed on HTL by interface modification for improving PCE, such as polymers poly (4-vinyl pyridine) (PVP), poly (N-90-heptadecanyl-2,7-carbazolealt-5,5-(40,70-di-2-thienyl-20,10,30-benzothiadiazole))PCDTBT), Interface engineering is widely applied in the one-step antisolvent deposition for elevating efficiency of the perovskite solar cells (PSCs). Herein, an alcohol-soluble small molecule, namely 2-mercaptoimidazole (MI), is inserted between the hole transport layer and perovskite layer to form a cross-linking bridge, which is built through: i) Coulomb interaction between the negatively charged MI and positively charged poly (3,4-ethylene dioxythiophene); ii) electrostatic interaction between imidazolium cation and iodide anion in perovskite. The cross-linking bridge can accelerate the hole transmission and inhibit interfacial recombination. Hence, by the optimum design of MI concentration, hysteresis-free devices with a hi...