A general approach is proposed to synthesize Janus polymer/inorganic composite nanosheets. Onto the amine-group-terminated side of the Janus inorganic nanosheets, initiators are covalently bonded. By a favorable grafting from initiator-terminated side, responsive polymers, for example PDEAEMA and PNIPAM, are synthesized by controlled polymerization for example ATRP or RAFT polymerization. Stable emulsions are easily formed in the presence of the Janus nanosheets, which can be easily de-emulsified by subtle changing physicochemical parameters, for example temperature and pH.