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Although electrostatic gating with liquid electrolytes has been thoroughly investigated to enhance electrical transport in two-dimensional (2D) materials, solid electrolyte alternatives are now actively being researched to overcome the limitations of liquid dielectrics. Here, we report direct growth of few-layer () molybdenum disulfide (), a prototypical 2D transition metal dichalcogenide (TMD), on lithium-ion solid electrolyte substrate by chemical vapor deposition (CVD), and demonstrate a transfer-free device fabrication method. The growth resulted in 5–10 μm sized triangular single crystals as confirmed by Raman spectroscopy, x-ray photoelectron spectroscopy, and scanning electron microscopy. Field-effect transistors (FETs) fabricated on the as-grown few-layer crystals show near-ideal gating performance with room temperature subthreshold swings around 65 mV/decade while maintaining an ON/OFF ratio …