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Chirality, a fundamental attribute of asymmetry, pervades in both nature and functional soft materials. In chiral material systems design, achieving global symmetry breaking of building blocks during assembly, with or without the aid of additives, has emerged as a promising strategy across domains including chiral sensing, electronics, photonics, spintronics, and biomimetics. We first introduce the fundamental aspects of chirality, including its structural basis and symmetry-breaking mechanisms considering free energy minimization. We particularly emphasize supramolecular assembly, such as through the formation of chiral liquid crystal phases. Next, we summarize processing strategies to control chiral symmetry breaking, exploiting external fields such as flow, magnetic fields, and templates. The final section discusses interactions between chiral molecular assemblies with circularly polarized (CP) light and electronic spin and their applications in CP light detectors, CP-spin-organic light-emitting diodes, CP displays, and spintronic devices based on the chirality-induced spin selectivity effect.