<p>The interplay between structural chirality and spin represents an emerging field with profound implications across multiple disciplines. As compared with organic chiral molecules and their organic-inorganic hybrids, all-inorganic chiral platforms remain underexplored, despite their potential as robust, tunable solid-state systems for the exotic chirality-entangled physics. Here we investigate chirality-driven light-matter-spin couplings in all-inorganic chiral heterostructures, comprising nanoscale chiral metal plasmonic cores and semiconductor quantum shells, without relying on extrinsic coupling to chiral molecules. We demonstrate that the structural handedness of the chiral Au core imprints chirality onto the CdS quantum shell, inducing significant spin polarization in the semiconductor. Moreover, observation of ultrafast dynamic chirality emerging in achiral CdS shells, driven by optical excitation of near-field chiral plasmons, suggests a transient chirality-driven effective magnetic field and provides a novel mechanism for ultrafast coherent spin manipulations. Our findings lay the groundwork for advancing solid-state chiral photonics and chiral spintronics, unraveling the potential of chirality-driven light-matter-spin interactions in quantum engineering.</p>