Nanopapers containing cellulose nanofibrils (CNFs) are an emerging and sustainable class of high performance materials. The diversification and improvement of the mechanical and functional property space critically depend on integration of CNFs with rationally designed, tailor-made polymers following bioinspired nanocomposite designs. Here we combine for the first time CNFs with colloidal dispersions of vitrimer nanoparticles (VP) into mechanically coherent nanopaper materials. Vitrimers are permanently cross-linked polymer networks that undergo temperature-induced bond shuffling through an associative mechanism and which allow welding and reshaping on the macroscale. The choice of low glass transition, hydrophobic vitrimers derived from fatty acids and polydimethylsiloxane (PDMS), and achieving dynamic reshuffling of cross-links through transesterification reactions enables excellent compatibility and covalent attachment onto the CNF surfaces. Moreover, the resulting films are ductile, stretchable and offer high water resistance. The success of imparting the vitrimeric polymeric behavior into the nanocomposite, as well as the curing mechanism of the vitrimer, is highlighted through thorough analysis of structural and mechanical properties. The dynamic exchange chemistry of the vitrimers enables efficient welding of two nanocomposite parts as characterized by good bonding strength during single lap shear tests. In the future, we expect that the dynamic character of vitrimers becomes a promising option for the design of mechanically adaptive bioinspired nanocomposites and for shaping and reshaping such materials.

Scaffold-based lattice-engineered 3D DNA origami is a powerful and versatile technique for the rational design and build-up of arbitrarily structured and monodisperse DNA-based 3D nanoobjects. Relying on the unsurpassed molecular programmability of sequence-specific DNA hybridization, a long DNA single strand (termed scaffold) is assembled with many short single-stranded oligomers (termed staples), which organize the scaffold into a 3D lattice in a single step, thereby leading to 3D nanoparticulate structures of the highest precision in high yields. Applications of 3D DNA origami are increasingly wide-spread and interface with numerous fields of sciences, for example, anisometric or anisotropically functionalized nanoparticles, fundamental investigations of superstructure formation, biomedicine, (bio)physics, sensors, and optical materials. This Minireview discusses the fundamentals and recent advances from structure formation to selected applications, with a mission to promote cross-disciplinary exchange.

Compartmentalization of chemical reactions inside cells are a fundamental requirement for life. Encapsulins are self‐assembling protein‐based nanocompartments from the prokaryotic repertoire that present a highly attractive platform for intracellular compartmentalization of chemical reactions by design. Using single‐molecule Förster resonance energy transfer and 3D‐MINFLUX analysis, we analyze fluorescently labeled encapsulins on a single‐molecule basis. Furthermore, by equipping these capsules with a synthetic ruthenium catalyst via covalent attachment to a non‐native host protein, we are able to perform in vitro catalysis and go on to show that engineered encapsulins can be used as hosts for transition metal catalysis inside living cells in confined space.

Compartmentalization of chemical reactions inside cells are af undamental requirement for life.E ncapsulins are self-assembling protein-based nanocompartments from the prokaryotic repertoire that present ahighly attractive platform for intracellular compartmentalization of chemical reactions by design. Using single-molecule Fçrster resonance energy transfer and 3D-MINFLUX analysis,weanalyzefluorescently labeled encapsulins on as ingle-molecule basis.F urthermore, by equipping these capsules with asynthetic ruthenium catalyst via covalent attachment to an on-native host protein, we are able to perform in vitro catalysis and go on to showt hat engineered encapsulins can be used as hosts for transition metal catalysis inside living cells in confined space.

3D DNA origami-based building blocks assemble reversibly to supracolloidal nanotubes using toehold-mediated strand displacement as probed by imaging and in situ FRET measurements.

The combination of supramolecular and covalent bonds enables a synergetic boost of mechanical properties for crustacean-mimetics using the molecular control mechanism.

Multicomponent self-assemblies cross-regulate their structures by exchange of molecular information using a metabolic network.

Block copolymer‐based polymersomes are important building blocks for the bottom‐up design of protocells and are considered advantageous over liposomes due to their higher mechanical stability and chemical versatility. Endowing both types of vesicles with capabilities for transmembrane transport is important for creating nanoreactor functionality and has been achieved by insertion of protein nanopores, even into comparably thick polymersome membranes. Still, the design space for protein nanopores is limited and higher flexibility might be accessible by de novo design of DNA nanopores, which have thus far been limited largely to liposome systems. Here, we introduce the successful insertion of two different 3D DNA origami nanopores into PMOXA‐b‐PDMS‐b‐PMOXA polymersomes, and confirm pore formation by dye influx studies and microscopy. This research thus opens the further design space of this versatile class of large DNA origami nanopores for polymersome‐based functional protocells.