nology to realize the advantages in making light-weight, fl exible, and large-scale solar panel by solution coating method. [ 26 ] From the aspect of mass production, fabrication process of PSC must meet the environment protection requirements. However, as a technology to produce green energy, the PSCs with the state-of-art effi ciencies were commonly fabricated by using hazardous organic solvents, [16][17][18] such as chlorobenzene (CB), o -dichlorobenzene (DCB), chloroform, diiodooctane (DIO) and so on. Since these chlorinated solvents may cause persistent pollution to environment and accumulative damage to animal and human health, researchers devoted great efforts to developing PSCs processed by environment-friendly solvents. [27][28][29][30] For instances, Chueh et al. used two nonchlorinated solvents, o -xylene (xylene) and trimethylbenzene, to process the polymer:fullerene derivative blend and obtained a PCE of 7.3%. [ 31 ] Chen et al. employed a halogen-free and aromatic-free solvent, 2-methyltetrahydrofuran to fabricate PSC devices and realized a PCE of 5.1% [ 32 ] Our group found that the blend of xylene and N -methylpyrrolidone (NMP) could replace the function of the blend of DCB and DIO in device fabrication and realized over 9% effi ciency; [ 29 ] more recently, we used the blend of anisole and diphenyl ether as the processing solvent to fabricate the PSCs and obtained a PCE of 8.37%. [ 33 ] According to these reported works, it can be concluded that although highboiling-point solvents or other treatments were used to modulate active layer morphology, effi ciencies of PSCs processed by environment-friendly solvents are still lower than the state-ofart effi ciency obtained from the PSCs processed by chlorinated solvents. Therefore, it is still a great challenge to fabricate highly effi cient PSCs by employing a single environment-friendly solvent without any further treatment.Low bandgap copolymers based on benzo[1,2b :4,5b ′]dithiophene (BDT) and thieno[3,4b ]thiophene (TT) units, namely PBDTTTs, have been successfully applied in fabricating highly effi cient PSCs. [34][35][36][37][38][39][40][41][42][43][44][45][46] However, it is worth noting that all highly effi cient PBDTTTs-based devices with PCE beyond 9% were achieved by using binary solvents. In this work, we fi rst proposed a novel solvent, 2-methylanisole (MA), as the processing solvent to fabricate PSCs based on PBDT-TS1, [ 37 ] a derivative of PBDTTTs, and realized a PCE of 9.67% without using any additives or posttreatments. As far as we know, this outstanding effi ciency is the highest among those of PSCs fabricated under additive-and posttreatment-free circumstance, and as similar as the reported results obtained from the halogenated DCB:DIO or the nonhalogenated xylene:NMP binary-solvent systems. More importantly, MA is a nonhalogenated, biodegradable chemical with low toxicity, and much safer than CB or DCB for mass production. For example, according to the hazards identifi cation on the Material Safety Data Sheet, there is only one h...