The utilization of deep blue phosphorescent materials in high-performance displays and solid-state lighting requires high quantum efficiencies and color purities. Here, we describe the preparation and luminescent properties of novel platinum triplet emitters featuring cyclometalated N-pyridyl-carbazole ligands functionalized with closo-monocarborane clusters [CB 11 H 12 ] − . All reported complexes were fully characterized by using standard small molecule techniques (UV−vis, cyclic voltammetry, nuclear magnetic resonance (NMR), high-resolution mass spectrometry (HRMS)), and their solid-state structures were elucidated by X-ray diffraction. These platinum phosphors emit in the blue region of the visible wavelength spectrum in both the solid and solution states. Complex 4a exhibits the highest luminous efficiency at λ em = 439 nm with a photoluminescent quantum yield (PLQY) of 60% by dispersing in a PMMA matrix. Electrochemical and computational studies of complexes 4a and 4b revealed that the blue phosphorescence originates mainly from intraligand 3 π → π* ( 3 ILCT) transitions with relatively small 3 MLCT mixing. A deep-blue OLED containing 4a as the light-emitting dopant was successfully fabricated using a solution-processed method, and the device exhibited blue photoluminescence with CIE coordinates of (0.17, 0.15) and a maximum external quantum efficiency (EQE max ) value of 6.2%. This article represents the pioneering study of a deep blue PhOLED using a Pt complex bearing a closo-monocarborane anion substituent, providing a new avenue into the preparation of novel triplet emitters based on boron-rich cluster anions.