Hydrophobic organo-compatible but low-capacitance dielectrics (10.5 nFcm(-2)), polystyrene-grafted SiO2 could induce surface-mediated large crystal grains of face-to-face stacked triethylsilylethynyl anthradithiophene (TES-ADT), producing more efficient charge-carrier transport, in comparison to mu m-sized pentacene crystals containing a face-to-edge packing. Low-voltage operating TES-ADT OFETs showed good device performance (mu(FET) approximate to 1.3 cm(2)V(-1)s(-1), Vth approximate to 0.5 V, SS approximate to 0.2 V), as well as excellent device reliability.