Layered transition metal dichalcogenides (TMDs) have received a great deal of attention due to fact that they have varied band gap, depending on their metal/chalcogen composition and on the crystal structure. Furthermore, these materials demonstrate great potential application in a myriad of electrochemical technologies. Heterogeneous electron transfer (HET) abilities of TMD materials toward redox-active molecules occupy a key role in their suitability for electrochemical devices. Herein, we introduce a promising biosensing strategy based on improved heterogeneous electron transfer rate of WS2, WSe2, and WTe2 nanosheets exfoliated using tert-butyllithium (t-BuLi) and n-butyllithium (n-BuLi) intercalators decorated with vertically aligned TiO2 nanoplatelets. By comparison of all the nanohybrids, decoration of TiO2 on t-BuLi WS2 (TiO2@t-BuLi WS2) results in the fastest HET rate of 5.39 × 10-3 cm s-1 toward ferri/ferrocyanide redox couple. In addition, the implications of decorating tungsten dichalcogenides (WX2) with TiO2 nanoplatelets in enzymatic biosensor applications for H2O2 detection are explored. TiO2@t-BuLi WS2 outperforms all other nanohybrid counterparts and is demonstrated to be an outstanding sensing platform in enzyme-based biosensor with wide linear range, low detection limit, and high selectivity. Such conceptually new electrocatalytic detection systems shall find the way to the next generation biosensors. ©