The physical and chemical properties of organic semiconductors are closely related to their aggregation structure. Tuning of aggregation structure and electrical property is important for the application in organic electronics. In this study, a facile way to tune the aggregation structure and electrical property of 2.6-diphenyl-anthracene (DPA) is realized by using the octadecyltrichlorosilane (OTS) modification layer with different density which is fabricated by controlling reaction temperature and time. Compared with low density OTS, DPA forms larger grain size, less grain boundaries, and better molecular ordering on high density OTS surface. As a result, the charge transporting mobility of DPA film on high density OTS surface is about two orders of magnitude higher than that on low density OTS surface. The tunable aggregation structure and electrical property of DPA demonstrated here would be meaningful for the application of DPA in organic electronics.