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The development of 2H–MoS2in supercapacitor is limited due to its poor conductivity and narrow interlayer spacing. The heterostructure assembly with conductive matrix is an effective means to improve conductivity, but the problem of narrow interlayer spacing still exists. Herein, by combining organic ion intercalation and heterostructure assembly, the narrow interlayer spacing and low conductivity of 2H–MoS2are optimized simultaneously. The synergistic effects are thereby obtaining, and the electrochemical advantages of different components in MoS2-PPy@Ti3C2Txare co-exerted. What's more, density functional theory (DFT) calculation is done to explore the kinetics storage mechanisms in MoS2samples, which shows that the polarity of MoS2has been enhanced for the introduction of Ti3C2TxMXene. This facilitated the mightier interface energy and extra capacitance. The current study smooths the path for structuring heterostructures on 2H–MoS2in the field of supercapacitors.