A sorbent in the form of a layered, non-porous perovskite is provided, wherein the sorbent can include parallel, alternating layers of an organic layer, including an ordered array of organic moieties capable of reacting with a gaseous halogen, and an inorganic layer, including a metal-halide sheet. Furthermore, each organic layer can be sandwiched between inorganic layers. Methods for capturing one or more halogens from a gas stream are also provided, wherein the methods can include contacting a gas stream with a sorbent in the form of a layered, non-porous perovskite, wherein the sorbent can include parallel, alternating layers of an organic layer, including an ordered array of organic moieties capable of reacting with a gaseous halogen, and an inorganic layer, including a metal-halide sheet. One or more halogens in the gas stream can react with either alkyne groups or alkene groups found in the organic layer of the sorbent.