We measure the spin Hall angle in Au layers of 5-100 nm thicknesses by spin pumping from Y3Fe5O12 epitaxial films grown by ultrahigh vacuum, off-axis sputtering. We observe a striking increase in the spin Hall angle for Au layers thinner than the measured spin diffusion length of 12.6 nm. In particular, the 5 nm Au layer shows a large spin Hall angle of 0.087, compared to those of 0.016 and 0.017 for the 50 and 100 nm Au layers, respectively, suggesting that the top surface plays a dominant role in spin Hall physics when the spin current is able to reach it. Other spin pumping related parameters, including Gilbert damping enhancement, interfacial spin mixing conductance, and spin current are also determined for Au layers of various thicknesses. Given the pervasive role of ultrathin films in electrical and spin transport applications, this result emphasizes the importance of considering the impact of the top surface and reveals the possibility of tuning critical spin parameters by film thickness.