For the better performance of organic thin-film transistors (TFTs), gate-insulator surface treatments are often applied. However, the origin of mobility increase has not been well understood because mobility-limiting factors have not been compared quantitatively. In this work, we clarify the influence of gate-insulator surface treatments in pentacene thin-film transistors on the limiting factors of mobility, i.e., size of crystal-growth domain, crystallite size, HOMO-band-edge fluctuation, and carrier transport barrier at domain boundary. We quantitatively investigated these factors for pentacene TFTs with bare, hexamethyldisilazane-treated, and polyimide-coated SiO2 layers as gate dielectrics. By applying these surface treatments, size of crystal-growth domain increases but both crystallite size and HOMO-band-edge fluctuation remain unchanged. Analyzing the experimental results, we also show that the barrier height at the boundary between crystal-growth domains is not sensitive to the treatments. The results imply that the essential increase in mobility by these surface treatments is only due to the increase in size of crystal-growth domain or the decrease in the number of energy barriers at domain boundaries in the TFT channel.