Some embodiments comprise membranes comprising a first layer comprising a porous graphene-based material; a second layer comprising a porous graphene-based material; a channel positioned between the first layer and the second layer, wherein the channel has a tunable channel diameter; and at least one spacer substance positioned in the channel, wherein the spacer substance is responsive to the environmental stimulus. In some cases, the membranes have more than two layers of porous graphene-based material. Permeability of a membrane can be altered by exposing the membrane to an environmental stimulus. Membranes can be used in methods of water filtration, immune-isolation, timed drug release (e.g., sustained or delayed release), hemodialysis, or hemofiltration.