Organic thin film transistors (OTFTs) have attracted intensive attention for potential applications in flexible displays, low-cost electronic papers. In recent years, my group has developed facile [X+1+Y] one-pot synthetic routes for fused thiophenes preparation, such as DTT (dithienothiophene), BTDT (benzothienodithiophene), TTA (tetrathienoacene), and PTA (pentathienothiophene). A few new fused-thiophene-based derivatives have been developed for OTFTs. For p-type materials development, we reported stable soluble BTDT-based materials with 0.65 cm2V-1s-1 mobility fabricated via a solution process. Recently, we have published two new soluble small molecules exhibited mobilities of 0.81 and 1.7 cm2V-1s-1, fabricated via a solution process. More recently, our new developed p-type small molecules have achieved high mobilities of 2.6 - 4.0 cm2V-1s-1. The later will be the Taiwan highest mobility small molecule via a solution process. For n-type materials development, we have developed a few new air-stable quinoidal molecules, for example, DTTQ exhibits ~0.45 cm2V-1s-1 mobility in air (AFM). Recently, we have developed two new soluble n-type small molecules exhibited mobilities of 0.77 and ~ 2.5 cm2V-1s-1, which will be the Taiwan highest n-type mobility small molecule via a solution process. Notably, these newly developed thiophene-based units are good building blocks and can be applied in OPV, 2PA, DSSC, and PSC. Our newly developed TTA-based chromophores exhibited high 2PA properties, up to 3000 GM, which is the highest performance of fused-thiophene-based 2PA chromophores. Our new developed TTA-based organic dyes exhibited PCE up to 11.2%, which also set a new highest record in Taiwan. Our new developed hole transporting layer (HTL) small molecules in Sn-based PSC (perovskite solar cell) exhibited 7.23 and 7.59 % PCE, both are one of the best HTLs for Sn-based PSC in the world. More recently, two of our new developed HTLs in Pb-based PSC exhibited 17.57 and 19.89 % PCE, hope the latter will be optimized to achieve a > 20% PCE very soon.Here in this project, we will continue modifying our newly-developed high-performance materials for their devices optimization and then published these good results. At the same time, new solution processable molecules will be developed for OTFT, OPV, and PSC. The optical/electronic performance of these new materials will be evaluated and optimized.