LAUSR

2D transition metal dichalcogenides are promising platforms for next‐generation electronics and spintronics. The layered Weyl semimetal (W,Mo)Te2 series features structural phase transition, nonsaturated magnetoresistance, superconductivity, and exotic topological physics. However, the superconducting critical temperature of the bulk (W,Mo)Te2 remains ultralow without applying a high pressure. Here, the significantly enhanced superconductivity is observed with a transition temperature as large as about 7.5 K in bulk Mo1−xTaxTe2 single crystals upon Ta doping (0 ≤ x ≤ 0.22), which is attributed to an enrichment of density of states at the Fermi level. In addition, an enhanced perpendicular upper critical field of 14.5 T exceeding the Pauli limit is also observed in Td‐phase Mo1−xTaxTe2 (x = 0.08), indicating the possible emergence of unconventional mixed singlet–triplet superconductivity owing to the inversion symmetry breaking. This work provides a new pathway for exploring the exotic superconductivity and topological physics in transition metal dichalcogenides.