The misfit layered compound ${\left(\text{PbS}\right)}_{1.11}{\mathrm{VS}}_2$ shows a complex interplay of structural modulation, disorder, and charge dynamics that leads to unconventional magnetic and transport properties. High resolution scanning transmission microscopy and temperature-dependent single crystal x-ray diffraction reveal short-range layer clustering, fractional layer sliding, diffuse scattering, and an appearance of new reflections below $T_{\text{s}}=220\mathrm{K}$, consistent with a continuous structural transition involving $c$-axis doubling and strengthened interlayer coupling. Below $T_{\text{s}}$, the resistivity increases by orders of magnitude and evolves into variable-range hopping; the data are most consistent with Efros-Shklovskii behavior driven by disorder-induced localization. The magnetoresistance is large, weakly anisotropic, and quadratic at low temperature, but at intermediate temperatures shows a complex shape, reflecting competing scattering and localization processes. Overall, the electronic state of ${\left(\text{PbS}\right)}_{1.11}{\mathrm{VS}}_2$ emerges from the combined action of structural modulation, disorder, and correlations with no single dominant mechanism governing its temperature-dependent electronic and magnetic behavior.

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• Anderson localization
• Electrical properties
• Magnetoresistance
• Metal-insulator transition
• Slidetronics
• Composite materials
• Disordered systems