This study investigated three newly developed high‐entropy cemented carbides (HECCs) with high‐entropy carbides (HECs) as the hard phase and Co as the binder. Accordingly, the interfacial wettability between HECs and Co was tuned by the changes in relative concentrations of the different metal components (e.g., W, Ta, and Ti) and C. Results demonstrate that the wettability between HECs and Co is dominated by the dissolution of HECs in Co, which determines the sintering behavior and hence the structure and performance of the materials. More specifically, the (W6Ta4Nb10Zr10Ti20)C50‐Co with lower W content has poorer interfacial wettability, leading to pores in the sintered HECC. The (W10Ta10Nb10Zr10Ti10)C50‐Co shows good interfacial wettability and strong resistance against grain boundary infiltration, owing to the formation of several atomic‐layer‐thick Co films between HEC grain boundaries. Reducing the C content facilitates the dissolution of HECs in Co, which can improve the interfacial wettability, but promotes the formation of η‐W3Co3C phase and embrittle the material. The (W10Ta10Nb10Zr10Ti10)C50‐Co with decent interfacial wettability exhibits a good balance of hardness (HV30 ∼1485), compressive strength (3316 MPa), and fracture toughness (10.9 MPa·m1/2). The work demonstrates a design strategy achieving optimized microstructure and mechanical performance in HECCs via tuning interfacial wettability.