Among various photovoltaic devices, dye-sensitized solar cells (DSSCs) are one of the most potentially clean and renewable energy conversion devices because of their low fabrication cost, environmentally friendly nature, and high power conversion efficiency. However, the use of rare metals such as Pt counter electrodes (CEs) is one of the major drawbacks of DSSC devices for broad real-life applications. In this regard, alternative materials to Pt CEs have been long sought for DSSCs employing both cobalt and iodine redox couples. Therefore, in this study, softtemplated tellurium-doped mesoporous carbons (Te-SMCs) were synthesized for the first time by the simple pyrolysis of PAN-b-PBA block copolymer in the presence of a tellurium precursor for replacing the Pt CE. To confirm the chemical composition and porosity, the as-prepared Te-SMC materials were evaluated by elemental analysis (XPS and EDS) and nitrogen sorption isotherms measurement. The as-prepared Te-SMC materials contained mainly mesopores and retained the three-dimensional hierarchical graphite-like structure with many defect sites. They displayed doping levels with nitrogen of 9.15 atom % and tellurium of 0.15 atom % and had a specific surface area of 540 m 2 g −1 . Therefore, these characteristics enabled the development of a high-performance CE in DSSCs with cobalt and iodine redox couples. As a result of its catalytic performance, Te-SMC exhibited outstanding electrocatalytic activity as well as a significantly improved electrochemical stability than those of Pt CE for both redox couples even after 1000 potential cycles. The results show that a maximum conversion efficiency of 11.64 and 9.67% could be achieved under one sun illumination (AM 1.5G) for SGT-021/Co(bpy) 3 2+/3+ -and N719/I − /I 3 − -based devices with Te-SMC CEs, and their power conversion efficiency is superior to the corresponding device with Pt CEs.