In nature, biogenic crystalline materials often incorporate surrounding biomacromolecules during crystallization, forming mechanically strengthened single crystal composites. Similarly, single-crystals grown from gel media can incorporate gel-networks, leading to a three-dimensional interpenetration structure without disrupting the long-range ordering. By virtue of the incorporation of gel networks, the habits of single crystal are changed and the intrinsic properties of the single crystal are improved. Moreover, functional nanomaterials can be introduced into single-crystals accompanied with the incorporation of gel-networks, endowing the crystalline host with non-intrinsic properties. As such, the incorporation of gel networks may expand the potential applications of the single crystal host. In this paper, we discuss the recent progress of regulating single crystal properties or functionalizing single-crystals by the incorporation of gel-networks, including the revolution of crystal morphologies, enhanced mechanical properties, regulation of semiconductor band gap and the functionalization of single crystals. Finally, the potential application of the gel-single crystal composite is predicted.