Epitaxially Grown Mechanically Robust 2D Thin Film of Secondary Interactions Led Molecularly Woven Material

Abstract Molecularly woven materials with striking mechanical resilience, and 2D controlled topologies like textiles, fishing nets, and baskets are highly anticipated. Molecular weaving exclusively apprehended by the secondary interactions expanding to laterally grown 2D self‐assemblies with retained crystalline arrangement is stimulating. The interlacing entails planar molecules screwed together to form 2D woven thin films. Here, secondary interactions led 2D interlaced molecularly woven material (2^°MW) built by 1D helical threads of organic chromophores twisted together via end‐to‐end CH···O connections, held strongly at inter‐crossing by multiple OH···N interactions to prevent slippage is presented. Whereas, 1D helical threads with face‐to‐face O–H···O connections sans interlacing led the non‐woven material (2^°NW). The polarity‐driven directionality in 2^°MW led the water‐actuated epitaxial growth of 2D‐sheets to lateral thin films restricted to nano‐scale thickness. The molecularly woven thin film is self‐healing, flexible, and mechanically resilient in nature, while maintaining the crystalline regularity is attributed to the supple secondary interactions (2^°).