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Abstract Au nanoclusters often demonstrate useful optical properties such as visible/near‐infrared photoluminescence, in addition to remarkable thermodynamic stability owing to their superatomic behavior. The smallest of the 8e⁻superatomic Au nanoclusters, Au₁₁, has limited applications due to its lack of luminescence and relatively low stability. In this work, we investigate the introduction of a single Pt dopant to the center of a halide‐ and triphenylphosphine‐ligated Au₁₁nanocluster, affording a cluster with a proposed molecular formula PtAu₁₀(PPh₃)₇Br₃. Electrochemical and spectroscopic analysis reveal an expansion of the HOMO–LUMO gap due to the Pt dopant, as well as relatively strong near‐infrared (NIR) photoluminescence which is atypical for an M₁₁cluster (λ_max= 700 nm, Φ = 1.88 %). The Pt dopant additionally boosted photostability; more than tenfold. Lastly, we demonstrate the application of the PtAu₁₀cluster's NIR photoluminescence in the detection of the nitroaromatic compound 2,4‐dinitrotoluene, with a limit‐of‐detection of 9.52 μM (1.74 ppm). The notable ability of a single central Pt dopant to unlock photoluminescence in a non‐luminescent nanocluster highlights the advantages of heterometal doping in the tuning of both the optical and thermodynamic properties of Au nanoclusters.