Environment‐Responsive Self‐Assembly and Coupled‐Network Effect in Dynamic Replicating Nucleopeptide Networks

The development of complex, adaptive behaviors in chemical systems hinges on the intricate coupling between reaction networks and self-organizing processes. Self-assembling networks, particularly those capable of self-replication, provide a unique platform for studying how molecular interactions drive temporally evolving, system-level behaviors. While environmental factors are known to shape the dynamic evolution of such networks, most studies have focused on static or single-class systems, such as isolated peptides or nucleic acids. This approach overlooks two critical dimensions of complexity: 1) nonlinear interspecies dynamics in multicomponent systems, and 2) inter-network coupling phenomena. Here, we investigate dynamic nucleopeptide networks exhibiting environment-responsive self-assembly, demonstrating how nucleobases and short peptides dynamically synergize under specific conditions to form organized, self-replicating structures. And we reveal how such networks orchestrate the interplay between cooperative and competitive species to achieve dynamic adaptation to environmental parameters (e.g., pH, temperature, and ionic strength). Furthermore, inspired by nucleobases' genetic information function, we utilized the base-specific recognition in nucleopeptide assemblies for hierarchical network coupling-transmitting environmental signals from stimulus-sensitive to stimulus-insensitive systems. These findings offer new insights into temporal and cross-network regulation of self-assembly and reaction dynamics, providing a framework for designing adaptive, life-like chemical systems that evolve and communicate with environmental signals.