In this work we report for the first time surface functionalization of 2D MoS2 with X (metals: Al, Cu, Sn, Ti) to develop a low-cost, ultra-selective biosensor array based Electronic Tongue (E-Tongue) for the detection of 4 vital neurological drugs in human saliva. The hydrothermally grown surface functionalized X-MoS2 was integrated onto a single 1 × 1 cm aluminium foil and contacts were defined using Cr electrodes. Detailed characterization revealed the formation of 2-H MoS2 and metal-X (Al, Cu, Sn, Ti)-functionalized MoS2 nanoflower like morphology decorated with nanoflake, nanorod, nanocube and nanostick structures, respectively. The response of the sensor array was recorded for aspirin, nicotine, caffeine and tramadol. Principal Component Analysis (PCA) was performed to reduce the dimension of numerous response data sets from all sensors and predict the likely possible response from various neurological drugs towards each sensor. Pattern-recognition analysis confirmed a definite pattern in response to respective functionalization and could efficiently differentiate neurological drugs from one another. Real-time analysis was performed using saliva samples for monitoring the therapeutic neurological drug concentration in the human body. Furthermore, the biosensor array was exposed to respective neurological drugs to study their sensitivity, selectivity, stability, reproducibility and adhesion onto the device. The strategy outlined can be used to develop lab-on-a-chip devices for the real-time detection of numerous bioanalytes in body fluids. © The Royal Society of Chemistry.