A Supramolecular Approach to Nanoscale Motion: Polymersome-Based Self-Propelled Nanomotors

[Image: see text] Autonomous micro- and nanoscale systems have revolutionized the way scientists look into the future, opening up new frontiers to approach and solve problems via a more bioinspired route. However, to achieve systems with higher complexity, superior output control, and multifunctionality, an in-depth study of the different factors that affect micro- and nanomotor behavior is crucial. From a fundamental perspective, the mechanical response of micro- and nanomotors still requires further study in order to have a better understanding of how exactly these systems operate and the different mechanisms of motion that can be combined into one system to achieve an optimal response. From a design engineering point of view, compatibility, degradability, specificity, sensitivity, responsiveness, and efficiency of the active systems fabricated to this point have to be addressed, with respect to the potential of these devices for biomedical applications. Nonetheless, optimizing the system with regards to all these areas is a challenging task with the micro- and nanomotors studied to date, as most of them consist of materials or designs that are unfavorable for further chemical or physical manipulation. As this new field of self-powered systems moves forward, the need for motor prototypes with different sizes, shapes, chemical functionalities, and architectures becomes increasingly important and will define not only the way active systems are powered, but also the methods for motor fabrication. Bottom-up supramolecular approaches have recently emerged as great candidates for the development of active structures that allow for chemical or physical functionalization, shape transformation, and compartmentalization, in a structure that provides a soft interface to improve molecular recognition and cell uptake. Our group pioneers the use of supramolecular structures as catalytically propelled systems via the fabrication of stomatocyte or tubular-shaped motors capable of displaying active motion in a substrate concentration-dependent fashion. This behavior demonstrates the potential of bottom-up assemblies for powering motion at the micro- or nanoscale, with a system that can be readily tuned and controlled at the molecular level. In this Account, we highlight the steps we have taken in order to understand and optimize the design of catalytically powered polymersome-based motors. Our research has been focused on addressing the importance of motor architecture, motion activation, direction control, and biological integration. While our work supports the feasibility of supramolecular structures for the design of active systems, we strongly believe that we are still in the initial stages of unveiling the full potential of supramolecular chemistry in the micro- and nanomotor field. We look forward to using this approach for the development of multifunctional and stimuli-responsive systems in the near future.