Unique optical, electrical, and mechanical properties of continuous semiconductor helices with nanoscale and mesoscale dimensions represent a previously unexplored materials platform for various applications requiring near-infrared (NIR) optical activity. However, current methods of their synthesis limit the spectrum of chiral geometries, charge transport, and spectral response. Furthermore, the requirements of nearly perfect enantioselectivity, high uniformity, and high yield need to be attained as well. Here, we show that continuous semiconductor helices with tunable spectral response and high monodispersity can be made via self-assembly of semiconductor nanoparticles (NPs). Unraveling the interdependent effects of solvent, pH, ligand density, and coordination bridges between NPs allowed us to maximize the chiral bias for face-to-face particle–particle interactions, control of the geometry of the helices, and increase assembly efficiency by 3 orders of magnitude. The self-limiting nature of NP association results in consistency of their geometries over the entire synthetic ensemble. The helices show chiroptical activity across a broad range of wavelengths from 300 to 1300 nm, and the maximum/sign of their polarization rotation in NIR part can be modulated by varying their pitch. The method described in this study can be extended to chiral semiconductor materials from a variety of other NPs and their combinations.

Sensors are widely used in various fields, among which flexible strain sensors that can sense minuscule mechanical signals and are easy to adapt to many irregular surfaces are attractive for structure health monitoring, early detection, and failure prevention in humans, machines, or buildings. In practical applications, subtle and abnormal vibrations generated from any direction are highly desired to detect and even orientate their directions initially to eliminate potential hazards. However, it is challenging for flexible strain sensors to achieve hypersensitivity and omnidirectionality simultaneously due to the restrictions of many materials with anisotropic mechanical/electrical properties and some micro/nanostructures they employed. Herein, it is revealed that the vision‐degraded scorpion detects subtle vibrations spatially and omnidirectionally using a slit sensillum with fan‐shaped grooves. A bioinspired flexible strain sensor consisting of curved microgrooves arranged around a central circle is devised, exhibiting an unprecedented gauge factor of over 18 000 and stability over 7000 cycles. It can sense and recognize vibrations of diverse input waveforms at different locations, bouncing behaviors of a free‐falling bead, and human wrist pulses regardless of sensor installation angles. The geometric designs can be translated to other material systems for potential applications including human health monitoring and engineering failure detection.

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