Controlling hydrogel surface wettability is of great importance in the viewpoint of engineering biomaterials that are in contact with cells and tissues. However, studies reporting how the hydrogel bulk properties would affect the surface is scarce, and thus it has been difficult to fabricate hydrogels with the desired properties. Also, there has been no effective method to elucidate this, due to the inhomogeneity introduced in the network structure of conventional hydrogels. Here we report our approach in elucidating the relationship between hydrogel physicochemical parameters and surface wettability by using Tetra-PEG gels, which are known to have homogeneous network structure. Specifically, the polymer volume fraction (φ) and the molecular weight (M W ) between the cross-links were controlled. The number of anions, cations, and ionic pairs introduced within the hydrogel, were also individually controlled. The surface wettability of the resulting hydrogels was then evaluated. Results showed that surface wettability is largely dependent on the concentration of charged groups that are introduced in the hydrogel bulk, especially those that are not paired and ionically stabilized. Our findings strongly support the fact that with conventional hydrogels, the correlation between surface wettability and its physicochemical properties had not been evaluated appropriately, and thus our insights will contribute significantly to accumulating further knowledge on controlling hydrogel surface wettability.