Abstract
Drug delivery plays a vital role in medicine and health, but the on-demand delivery of large-sized drugs using stimuli-triggered carriers is extremely challenging. Most present capsules consist of polymeric dense shells with nanosized pores (<10 nm), thus typically lack permeability for nano/microparticle drugs. Here, a pinecone-inspired smart microcage with open network shells, assembled from cellulose nanofibrils (CNFs), is reported for nano/microparticle drug delivery. The approach allows the nanoarchitectured, functionalized CNFs to assemble into mechanically robust, haystack-like network shells with tunable large-through pores and polypeptide-anchored points on a large scale. Such open network shells can intelligently open/close triggered by lesion stimuli, making the therapy "always on-demand." The resulting pinecone-inspired microcages exhibit integrated properties of superior structural stability, superhydrophilicity, and pH-triggered, smart across-shell transport of emerging antimicrobial silver nanoparticles and bioactive silicate nanoplatelets (sizes of >100 nm), which enable both extraordinary anti-infection and bone regeneration. This work provides new insights into the design and development of multifunctional encapsulation and delivery carriers for medical and environmental applications.