Polymeric lamination of functional nanoparticles (NPs) is achieved mainly by covalent conjugation or physical adsorption. However, it is hard to control the recovery of bioactivity/toxicity of functional NPs, thereby exhibiting limited applications in areas. Herein, we report the construction of hyaluronic acid (HA) laminated, inherently toxic methylviologen (MV) nanoparticles, HA-MV-NPs, via ternary host-guest complexation between cucurbit[8]uril (CB[8]), trans-azobenzene conjugated HA, and MV-functionalized polylactic acid nanoparticle (MV-NPs). The non-specific toxicity of MV-NPs has been effectively shielded by HA lamination, which was demonstrated in cells, zebrafish, and mouse models. CB[8]-based host-guest interactions offer the resulting materials additional modalities (such as UV irradiation) to precisely remove HA lamination on demand, thereby endowing materials with the capability of selective decoating-induced activation (DIA) for user-friendly herbicide, selective antibacterial agent and in vivo controlled release. This work offers facile supramolecular coating strategies to tame and precisely control the bioactivity and toxicity of certain nanomaterials.