Inflammation is one of the most common pathological processes involved in numerous diseases. Thus, bioimaging of inflammation is of great significance for the diagnosis and treatment of a variety of inflammatory diseases. Herein, for the first time, we report a supramolecular luminol-AIEgen nanoparticle (SLA NP)-based bioluminescent probe for deep-tissue-inflammation imaging. SLA NPs were facilely fabricated by anchoring adamantane-luminol (AdLum) onto NPs derived from AIEgen-cucurbit[7]uril (AIECB[7]) via CB[7]-Ad host-guest interactions. The designed SLA NPs are capable of efficient bioluminescence resonance energy transfer (BRET) from luminol (donor) to AIEgen (acceptor), enabling deep-tissue penetration and fluorescent imaging. SLA NPs possess uniform particle size and excellent stability and biocompatibility for in vitro and in vivo inflammation imaging, superior to commercial luminol. This work not only demonstrates the enhanced deep-tissue-inflammation imaging of luminol via its BRET pairing with AIEgen NPs but also offers important new insights into the construction of luminol-AIEgen BRET pairs through host-guest complexation.