However, the large ionic radius of K + (2.76 Å) is unfavorable for its insertion into anode materials, resulting in a relatively low specific capacity and poor rate performance. [2] To meet the requirements of the energy storage technologies for rechargeable KIBs, the development of high-performance materials with high capacity and favorable reliability has become increasingly urgent. [3] 2D-layered transition metal dichalcogenides (TMDs) with a formula of MX 2 (M = Mo, W, V, Ta, and Ti; X = S, Se, and Te) have attracted significant interest because of their highly accessible surface area, fast charge-transfer kinetics, and the undercoordinated edge sites of layered TMDs, which can act as extra adsorption sites for metal ions. [4] Especially, 2D TMDs with expanded interlayer spacing will be highly desired to accommodate the largesized potassium ions (K + ) for the fast K + diffusion in high-performance KIBs. [5] As a typical 2D TMD, molybdenum disulfide (MoS 2 ) with distinctive semiconductor properties has gained special attention. [6] 2D MoS 2 shows a direct bandgap in multiple phases: a semiconducting 2D hexagonal phase (2H phase) with a trigonal prismatic crystal structure (2H-MoS 2 ), a metallic 1T phase with a triclinic crystal structure (1T-MoS 2 ) and edge-sharing octahedra, and a distorted triclinic phase (1T′-MoS 2 ), [7] offering broad application potentials in diversified optical and electronic devices. [8] Indeed, Efficient exfoliations of bulk molybdenum disulfide (MoS 2 ) into few-layered nanosheets in pure phase are highly attractive because of the promising applications of the resulted 2D materials in diversified optoelectronic devices. Here, a new exfoliation method is presented to prepare semiconductive 2D hexagonal phase (2H phase) MoS 2 -cellulose nanocrystal (CNC) nanocomposites using grinding-promoted intercalation exfoliation (GPIE). This method with facile grinding of the bulk MoS 2 and CNC powder followed by conventional liquid-phase exfoliation in water can not only efficiently exfoliate 2H-MoS 2 nanosheets, but also produce the 2H-MoS 2 /CNC 2D nanocomposites simultaneously. Interestingly, the intercalated CNC sandwiched in MoS 2 nanosheets increases the interlayer spacing of 2H-MoS 2 , providing perfect conditions to accommodate the large-sized ions. Therefore, these nanocomposites are good anode materials of potassium-ion batteries (KIBs), showing a high reversible capacity of 203 mAh g −1 at 200 mA g −1 after 300 cycles, a good reversible capacity of 114 mAh g −1 at 500 mA g −1 , and a low decay of 0.02% per cycle over 1500 cycles. With these impressive KIB performances, this efficient GPIE method will open up a new avenue to prepare pure-phase MoS 2 and promising 2D nanocomposites for highperformance device applications.