Hydrogels, formed through crosslinking of hydrophilic polymer chains, represent a class of materials that are capable of holding large volumes of water. Here we report a novel class of hydrophobic hydrogels that can free-float on the surface of different aqueous media by coating conventional hydrogels with a layer of hydrophobic microparticles. We further demonstrate that these floating hydrogel-based devices can be used for sensing applications on liquid surfaces such as the construction of floating pH meters. Moreover, we demonstrate that the floating hydrogels present high mobility with excellent self-assembling property on the surface of water. Importantly, the floating systems reserved the intrinsic biocompatibility of the core hydrogels, enabling microengineering of floating tissue constructs. It is expected that these floating hydrophobic hydrogel-based devices will likely find widespread applications including but not limited to sensing, tissue engineering, and biomedicine.